Millicharged particles (mCPs) are hypothesized particles possessing an electric charge that is a fraction of the charge of the electron. We report a search for mCPs with charges > ∼ 10 −4 e that improves sensitivity to their abundance in matter by roughly two orders of magnitude relative to previous searches. This search reaches abundances predicted for the accumulation of relic dark matter mCPs with masses between 1-100 GeV in terrestrial matter, corresponding to a gap in parameter space that is beyond the reach of previous searches from accelerators, colliders, cosmicray experiments, and cosmological constraints. Our results also set a limit on the deviation from zero of the sum of the charges of the proton, neutron and electron at the level of ∼ 3 × 10 −19 e. While these constraints are two orders of magnitude weaker than the best existing tests of matter neutrality, the sensitivity demonstrated here is sufficient to exceed existing techniques if backgrounds can be further reduced in future searches.