The electrochemical performance of zinc particles with 250 μm and 30 μm diameters, coated with Bi2O3-Li2O-ZnO glass is investigated and compared with noncoated zinc particles. Galvanostatic investigations were conducted in the form of complete discharge and charging cycles in electrolyte excess. Coated 30 μm zinc particles provide the best rechargeability after complete discharge. The coatings reached an average charge capacity over 20 cycles of 113 mAh/g compared to the known zero rechargeability of uncoated zinc particles. Proposed reasons for the prolonged cycle life are effective immobilization of discharge products in the glass layer and the formation of percolating metallic bismuth and zinc phases, forming a conductive network through the glass matrix. The coating itself is carried out by mechanical ball milling. Different coating parameters and the resulting coating quality as well as their influence on the passivation and on the rechargeability of zinc–glass composites is investigated. Optimized coating qualities with respect to adhesion, homogeneity and compactness of the glass layer are achieved at defined preparation conditions, providing a glass coating content of almost 5 wt % for 250 μm zinc particles and almost 11 wt % for 30 μm zinc particles.