The resin-bonded spherical diamond wheel is widely used in arc envelope grinding, where the demands for form accuracy are high and the form truing process is challenging. In this paper, on-machine precision form truing of the resin-bonded spherical diamond wheel is accomplished by using a coarse-grained diamond roller, and in-situ measurement of the form-truing error is conducted through a laser scan micrometer. Firstly, a novel biarc curve-fitting method is proposed based on the in-situ measurement results to calculate the alignment error between the diamond roller and the spherical diamond wheel. Then, on-machine precision form truing of a D46 resin-bonded spherical diamond wheel is completed after alignment error compensation. The in-situ measurement results show that the low-frequency form-truing error is approximately 5 μm. In addition, the actual form-trued diamond wheel has been employed in grinding a test specimen, and the resulting form accuracy is approximately 1.6 μm without any compensation. The ground surface profile shared similar characteristics with the roller-trued diamond wheel profile, confirming that the diamond roller truing and in-situ measurements methods are accurate and feasible.