Let $(X,d)$ be a complete separable metric space (Polish space) with a Borel probability measure $\mu$. Given $\varepsilon_1, \varepsilon_2 > 0$ can one find a finite set of disjoint open balls $B_1,\ldots, B_n$ of diameter $< \varepsilon_1$ such that $\mu(B_1) + \ldots + \mu(B_n) > 1-\varepsilon_2$?
I am embarrassed I am asking this. I hope it is not as trivial as I fear!
After a lot of searching on the web, the general answer is no.
(Notice, this also applies to disjoint open balls (replacing $< 1/2$ with $\leq 1/2$) by slightly shrinking the open balls to be closed.) This is Example 4.49 in Counterexamples in Probability and Real Analyisis. (It is great to know such a book exists!) They cite Davies, "Measures are not approximable or specifiable by means of balls" 1971. In that paper Davies shows an even more interesting theorem.
Hence on $\Omega^*$, the measures of the balls alone don't determine the structure of the measure. (Instead one needs to know the measures of the finite unions of balls as well.)
Positive results:
For the space $[0,1]^n$ with the Lebesgue measure, such a covering theorem does exist via the Vitali covering theorem.
The same is true for any Borel probability measure $\mu$ on $\mathbb{R}^n$ via the Besicovitch covering theorem.
Davies also mentions that the result holds when the space is finite dimensional in some sense.