A two-dimensional layered manganese(II) pyrophosphate, 2[Mn3(P2O7)2(H2O)2] (1), has been synthesized hydrothermally. Its structure is determined by single-crystal X-ray diffraction analysis. Its structure is built up by MnO6 octahedra and P2O7 units, with ammonium NH4+ cations residing in the interlayer regions. The manganese pyrophosphate layer consists of infinite chains of cis and trans edge sharing MnO6 octahedra linked by P2O7 units. Magnetic susceptibility measurements show that this compound exhibits ferrimagnetic-like ordering below 3.2 K. Further study shows that there are two possible superexchange pathways via the oxygen anions in Mn2+ ions. Owing to the different bridging modes of O2-, the competition between ferromagnetic interactions and antiferromagnetic interactions in Mn2+ ions results in the ferrimagnetic behavior of 1.