Covalently bonded carbon nitride materials (e.g., g-C3N4) have numerous potential applications ranging from semiconductors to fuel cells. But their solubility is poor, which makes characterization and processing difficult. Moreover, the chemistry of the as-synthesized carbon nitrides has been widely neglected. Here we report that some of these handicaps might be overcome by a controllable and reversible protonation. It was found that protonation not only provides better dispersion and exposes a high surface area for g-C3N4 but also enables an adjustment of electronic band gaps and higher ionic conductivity. Recovery or deprotonation toward the original g-C3N4 could be obtained by simple heating, which enables improved sintering but also a potential preservation of the higher surface area of the protonated material. This proton-enhanced sintering process allowed for the first time direct measurement of the photoconductivity of the material. By aid of protonation, other promising g-C3N4 based hybrid composites could also be facilely obtained by simple counteranion exchange.