An ultraviolet detector is demonstrated through a whole‐wafer, thin diamond film transfer process to realize the heterojunction between graphene and microcrystalline diamond (MCD). Conventional direct transfer processes fail to deposit graphene onto the top surface of the MCD film. However, it is found that the 2 µm thick MCD diamond film can be easily peeled off from the growth silicon substrate to expose its smooth backside for the graphene transfer process for high‐quality graphene/MCD heterojunctions. A vertical graphene/MCD/metal structure is constructed as the photodiode device using graphene as the transparent top electrode for solar‐blind ultraviolet sensing with high responsivity and gain factor. As such, this material system and device architecture could serve as the platform for next‐generation optoelectronic systems.