$\DeclareMathOperator{\Sq}{Sq}\newcommand{\Z}{\mathbb{Z}}$The short version is that every cohomology operation can be interpreted as a Bockstein operator for an "exact sequence" (read: fiber sequence) of grouplike $E_\infty$ spaces.

Any cohomology operation $\delta:H^*(-;A)\Rightarrow H^{*+k}(-;B)$ such as $\Sq^i$ gives a morphism of Eilenberg-MacLane spectra $f_\delta:HA\to \Sigma^k HB$. You can take the fiber of $f_\delta$ to obtain a spectrum $F$ which defines a generalized cohomology theory $E_F^*:X\mapsto \pi_{-*} F^X$, and there is a resulting long exact sequence
$$
\dots\to E_F^i(X)\to H^i(X;A)\xrightarrow{\delta}H^{i+k}(X;B)\to E_F^{i+1}(X)\to\dots
$$
If $\delta = \Sq^1$, the fiber is again an Eilenberg-MacLane spectrum (namely $F\simeq H\Z/4$). If the degree of $\delta$ is bigger than $1$, it will have two non-zero homotopy groups, namely $A$ in degree $0$ and $B$ in degree $k-1$.

The connection to the crossed modules you mention is that applying the functor $\Omega^{\infty-1}$ to the fiber of $\Sq^2$ gives rise to a $2$-group, i.e. a homotopy type $X$ whose homotopy groups vanish outside degrees $1$ and $2$. As you mention, these are classified by the two groups $A = \pi_1(X),B = \pi_2(X)$, the action of the former on the latter, and a $k$-invariant in $H^3(A;B)$, which together can be packaged into the datum of a crossed module. However, these deloop once if and only if the action is trivial and the $k$-invariant vanishes. It is still possible to find reasonably easy algebraic models for spaces whose homotopy groups vanish outside degrees $k$ and $k+1$ (given by braided ($k=2$) and symmetric ($k\ge 3$) monoidal Picard (every object has a tensor inverse) groupoids), although I do not know a definition of $\Sq^2$ in this language.

# Questions in the comments

 1. You already discuss the resulting cohomology operation in the case that the action of $A$ on $D$ is trivial. For the general case, one first construts a natural transformation from $H^1(-;A)$ to local systems: $H^1(-;A)$ are isomorphism classes of $A$-principal bundles, and this natural transformation sends a principal bundle $P$ to $P\times_A D$. A cohomology class in $H^k(A;D)$ then gives a natural transformation from $H^1(-;A)$ to $H^k$ of this local system, by the same construction as in the trivial case.
  2. Yes, for a $(2,3)$-type $X$ the $2$-group $\Omega X$ is split, i.e. the action of $\pi_1(\Omega X)\cong \pi_2(X)$ on $\pi_2(\Omega X)\cong \pi_3(X)$ is trivial (this can be shown by the Eckmann-Hilton argument) and the $k$-invariant vanishes.
  3. For degree $2$ cohomology operations, there is in fact a complete classification (compare https://mathoverflow.net/questions/24754/cohomology-of-the-eilenberg-maclane-spaces-kg-n and the cited references): operations $H^2(-;A)\to H^4(-;B)$ are given by quadratic functions $q:A\to B$ (i.e. such that $q(x+y) - q(x) - q(y)$ is bilinear and $q(kx) = k^2q(x)$), and the resulting cohomology operation is given by a suitable version of the [Pontryagin square][1]. For $k\ge 3$, operations are in bijection with linear maps from $A\otimes \Z/2$ to $B$ (observe that such a *linear* map is also quadratic by the "freshman's dream"), and the resulting cohomology operation is the composition

$$
H^*(-;A)\to H^*(-;A\otimes Z/2)\xrightarrow{\Sq^2} H^{*+2}(-;A\otimes\Z/2)\to H^{*+2}(-;B)
$$

The relation to Picard groupoids is a consequence of the [Homotopy hypothesis][2], and given a braided Picard groupoid $C$, you can associate to it its abelian group $\pi_0 C$ of isomorphism classes and the (abelian!) group $\pi_1 C$ of automorphisms of the unit $1$, together with the map $q: \pi_0 C\to \pi_1 C$ which sends $x$ to the composition

$$
1\cong x\otimes x^{-1}\xrightarrow{\beta_{x,x^{-1}}} x^{-1}\otimes x\cong 1
$$

It's a fun exercise to show that $q$ is quadratic in the above sense. It is not straightforward to give an inverse to this construction, i.e. construct the braided Picard groupoid from the quadratic map; for a reference in the symmetric setting, see [Cegarra, A. M.; Khmaladze, E., Homotopy classification of graded Picard categories, Adv. Math. 213 (2007)][3].

A chain level representative of $\Sq^2$ (and higher Steenrod squares) can be found in [Ralph M. Kaufmann, Anibal M. Medina-Mardones. Cochain level May-Steenrod operations][4].


  [1]: https://encyclopediaofmath.org/wiki/Pontryagin_square
  [2]: https://en.wikipedia.org/wiki/Homotopy_hypothesis
  [3]: https://doi.org/10.1016/j.aim.2007.01.015
  [4]: https://arxiv.org/abs/2010.02571v4