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For machining of hard and brittle materials, iron electrodeposit is a kind of matrix material with potential advantages for manufacture of diamond tools. Aiming at the problem of difficult codeposition of diamond in iron deposit, this paper adopts orthogonal design of experiment to study the effects of solution pH value, cathodic current density, alkylphenol polyoxyethylene (10) ether (OP-10) concentration and ammonium chloride concentration on codeposition of diamond, and then Fe-based diamond bits were fabricated and drilling tests in granite were carried out. The results show that pH value, cathodic current density, OP-10 concentration and ammonium chloride concentration all have statistically significant effect on codeposition of diamond in iron deposit, whose contributions to the variance of the weight of codeposited diamond are 37.45%, 32.05%, 13.13% and 12.38%, respectively. The result of drilling test indicates that Fe-based diamond bit can achieve much higher penetration rate than common Ni-based diamond bit.