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Regarding Charles Rezk's second question:

This leaves open the possibility that there are topological manifolds which do not admit any PL-structure but are still homeomorphic to some simplicial complex. Is this possible?

For dimension 4, it follows from the Poincare conjecture that a 4-manifold is triangulable iff smoothable (which is also equivalent to having PL structure for dimension <8). See Problem 3 of http://www.maths.ed.ac.uk/~aar/haupt/sandro.pdf. Also see this presentation.

For dimension >4, Springer Online Reference Works claims that "the imbedding $PL \subset TRI$ is also irreversible in the same strong sense (there exist polyhedral manifolds of dimension $\geq 5$ that are homotopy inequivalent to any PL-manifold)", but gives no examples. In this presentation it is stated that "All oriented closed 5-manifolds triangulable", so I think among them there may be some with nontrivial KS invariant and hence cannot bear PL structure.

In addition, This book (p.168, Theorem 18.4) seems to contain a result that strengthens the one mentioned in Paul's answer.

Added: This paper (22.5. Example) explicitly gives an example of "A topological manifold which is homeomorphic to a polyhedron but does not admit any PL structure".

Regarding Charles Rezk's second question:

This leaves open the possibility that there are topological manifolds which do not admit any PL-structure but are still homeomorphic to some simplicial complex. Is this possible?

For dimension 4, it follows from the Poincare conjecture that a 4-manifold is triangulable iff smoothable (which is also equivalent to having PL structure for dimension <8). See Problem 3 of Fragments of geometric topology from the sixties by Sandro Buoncristiano. Also see the presentation From Triangulations to 4-Manifolds: In Honor of Takao Matumoto’s 60^th Birthday by Ron Stern.

For dimension >4, Springer Online Reference Works claims that "the imbedding $PL \subset TRI$ is also irreversible in the same strong sense (there exist polyhedral manifolds of dimension $\geq 5$ that are homotopy inequivalent to any PL-manifold)", but gives no examples. In Ron Stern's presentation it is stated that "All oriented closed 5-manifolds triangulable", so I think among them there may be some with nontrivial KS invariant and hence cannot bear PL structure.

In addition, the book Lectures on the Topology of 3-manifolds: An Introduction to the Casson Invariant (p.168, Theorem 18.4) by Nikolai Saveliev seems to contain a result that strengthens the one mentioned in Paul's answer.

Added: The paper Piecewise linear structures on topological manifolds (22.5. Example) by Yuli B. Rudyak explicitly gives an example of "A topological manifold which is homeomorphic to a polyhedron but does not admit any PL structure".

Regarding Charles Rezk's second question:

This leaves open the possibility that there are topological manifolds which do not admit any PL-structure but are still homeomorphic to some simplicial complex. Is this possible?

For dimension 4, it follows from the Poincare conjecture that a 4-manifold is triangulable iff smoothable (which is also equivalent to having PL structure for dimension <8). See Problem 3 of http://www.maths.ed.ac.uk/~aar/haupt/sandro.pdf. Also see this presentation.

For dimension >4, Springer Online Reference Works claims that "the imbedding $PL \subset TRI$ is also irreversible in the same strong sense (there exist polyhedral manifolds of dimension $\geq 5$ that are homotopy inequivalent to any PL-manifold)", but gives no examples. In this presentation it is stated that "All oriented closed 5-manifolds triangulable", so I think among them there may be some with nontrivial KS invariant and hence cannot bear PL structure.

In addition, This book (p.168, Theorem 18.4) seems to conatain a result that strengthens the one mentioned in Paul's answer.

Added: This paper (22.5. Example) explicitly gives an example of "A topological manifold which is homeomorphic to a polyhedron but does not admit any PL structure".

Regarding Charles Rezk's second question:

This leaves open the possibility that there are topological manifolds which do not admit any PL-structure but are still homeomorphic to some simplicial complex. Is this possible?

For dimension 4, it follows from the Poincare conjecture that a 4-manifold is triangulable iff smoothable (which is also equivalent to having PL structure for dimension <8). See Problem 3 of http://www.maths.ed.ac.uk/~aar/haupt/sandro.pdf. Also see this presentation.

For dimension >4, Springer Online Reference Works claims that "the imbedding $PL \subset TRI$ is also irreversible in the same strong sense (there exist polyhedral manifolds of dimension $\geq 5$ that are homotopy inequivalent to any PL-manifold)", but gives no examples. In this presentation it is stated that "All oriented closed 5-manifolds triangulable", so I think among them there may be some with nontrivial KS invariant and hence cannot bear PL structure.

In addition, This book (p.168, Theorem 18.4) seems to contain a result that strengthens the one mentioned in Paul's answer.

Added: This paper (22.5. Example) explicitly gives an example of "A topological manifold which is homeomorphic to a polyhedron but does not admit any PL structure".

Regarding Charles Rezk's second question:

This leaves open the possibility that there are topological manifolds which do not admit any PL-structure but are still homeomorphic to some simplicial complex. Is this possible?

For dimension 4, it follows from the Poincare conjecture that a 4-manifold is triangulable iff smoothable (which is also equivalent to having PL structure for dimension <8). See Problem 3 of http://www.maths.ed.ac.uk/~aar/haupt/sandro.pdf. Also see this presentation.

For dimension >4, Springer Online Reference Works claims that "the imbedding $PL \subset TRI$ is also irreversible in the same strong sense (there exist polyhedral manifolds of dimension $\geq 5$ that are homotopy inequivalent to any PL-manifold)", but gives no examples. In this presentation it is stated that "All oriented closed 5-manifolds triangulable", so I think among them there may be some with nontrivial KS invariant and hence cannot bear PL structure.

In addition, This book (p.168, Theorem 18.4) seems to conatain a result that strengthens the one mentioned in Paul's answer.

Regarding Charles Rezk's second question:

This leaves open the possibility that there are topological manifolds which do not admit any PL-structure but are still homeomorphic to some simplicial complex. Is this possible?

For dimension 4, it follows from the Poincare conjecture that a 4-manifold is triangulable iff smoothable (which is also equivalent to having PL structure for dimension <8). See Problem 3 of http://www.maths.ed.ac.uk/~aar/haupt/sandro.pdf. Also see this presentation.

For dimension >4, Springer Online Reference Works claims that "the imbedding $PL \subset TRI$ is also irreversible in the same strong sense (there exist polyhedral manifolds of dimension $\geq 5$ that are homotopy inequivalent to any PL-manifold)", but gives no examples. In this presentation it is stated that "All oriented closed 5-manifolds triangulable", so I think among them there may be some with nontrivial KS invariant and hence cannot bear PL structure.

In addition, This book (p.168, Theorem 18.4) seems to conatain a result that strengthens the one mentioned in Paul's answer.

Added: This paper (22.5. Example) explicitly gives an example of "A topological manifold which is homeomorphic to a polyhedron but does not admit any PL structure".