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Nate Eldredge
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Stealing an answer from "user940" on Math.SE, the answer is yes, such a measures can exist, at least for closed balls. In the paper

Davies, Roy O., Measures not approximable or not specifiable by means of balls, Mathematika, Lond. 18, 157-160 (1971). ZBL0229.28005.

the author constructs a compact metric space $X$ and two distinct Borel probability measures $\mu_1, \mu_2$ that agree on every closed ball. (They must therefore also agree on open balls, because an open ball is a countable increasing union of closed balls.) Taking $\mu = \mu_1 - \mu_2$ provides your desired signed measure.

Nate Eldredge
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