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A single-step doping method capable of high resolution n- and p-type doping of large area graphene is presented. Thin films of hydrogen silsesquoxane on exfoliated graphene are used to demonstrate both electron and hole doping through control of the polymer cross-linking process. This dual-doping is attributed to the mismatch in bond strength of the Si–H and Si–O bonds in the film as well as out-gassing of hydrogen with increasing cross-linking. A high-resolution graphene p-n junction is demonstrated using this method.