A new layered aluminophosphate, [C6N3H17][Al2(HPO4)(PO4)2] (denoted AlPO-CJ21), has been prepared in an alcoholic system by the use of N-(2-aminoethyl)-piperazine (AEPP) as the template. Its inorganic layer containing a series of bridged six-membered rings (MRs) is a new type of 4.6-net sheet built up from AlO4, PO2(OH)(=O), and PO3(=O) tetrahedra. Interestingly, inorganic helical chains of right- or left-handedness are presented in the aluminophosphate layers, and fascinating hydrogen-bonded helices are self-assembled under solvothermal conditions between organic templates and inorganic sheets via strong hydrogen bondings of O...N atoms. Crystal data: monoclinic, P2(1) (No. 4), a = 10.069(2) A, b = 8.0875(16) A, c = 10.598(2) A, beta = 94.71(3) degrees, z = 2, R(1) = 0.0325 [I > 2sigma(I)], and wR(2) = 0.0807 (all data); Flack parameter: 0.03.