As far as we are concerned, the phenomenon of Ni2+ luminescence in tetrahedral coordination has not been reported. For the first time, a new NIR phosphor Ca2GeO4:Ni2+ is developed in this work. It is found that the NIR emission from this phosphor is a sharp peak attributed to the unusual Ni2+-occupied GeO4 site in the lattice, instead of the conventional broadband luminescence of Ni2+ in the octahedrally coordinated site. Crystal-field analysis has been applied, and the parameters Dq, B, and Δ are calculated to reveal the relationship between the emission profile and the crystal field strength. The optimal Ni2+ doping concentration is found to be 1%. Ca2GeO4:Ni2+ provides an efficient sharp-line (fwhm = 16 nm) emission centered at 1164 nm which originates from the 1T2 → 3T1 transition with an internal quantum efficiency of 23.1% and a decay lifetime of about 300 μs. This work could provide some new insights to explore novel NIR luminescent materials based on transition-metal elements.