Three open‐framework gallium phosphates [C6H16N2][Ga(HPO4)(PO4)] (1), {H[C6H16N2]2[Ga7(OH)2(PO4)8]} (2), and {H[C4H12N2]2[Ga7(OH)2(PO4)8]·2H2O} (3) were solvothermally synthesized in the presence of 2,6‐dimethylpyrazine, N‐ethylpiperazine, and piperazine as templates, respectively. Compound 1 possesses an infinite one‐dimensional chain structure connected by hydrogen‐bond interactions to generate a 3D supramolecular framework. Compounds 2 and 3 show similar inorganic framework structures, which may be viewed as the assembly of a secondary building unit (SBU), Ga6P8 containing two GaO4, two GaO5, two GaO6 as well as eight PO4 groups. The SBUs are linked with each other by vertex‐sharing oxygen atoms to form 2D sheets, which are further connected by GaO4 tetrahedra to result in the final 3D open‐framework with left‐ and right‐handed helical chains. In these materials, the well‐ordered organic species reside in the voids of structures and interact with the framework by way of hydrogen bonds.