A series of Tb(3+)-activated NaLi2PO4 novel nano-crystalline phosphors was synthesized by the solution combustion method. The prepared Na(1-x)Li2PO4:xTb(3+) (0.01 ≤ x ≤ 0.1) phosphors crystallized in the orthorhombic crystal structure. Its effective absorption in the near ultraviolet range allowed highly efficient green emission. The Na(1-x)Li2PO4:xTb(3+) phosphors showed characteristic (5)D4 --> (7)FJ (J = 3, 4, 5, and 6) transitions of Tb(3+), i.e., (5)D4 --> (7)F6 (488 nm), (5)D4 --> (7)F5 (545 nm), (5)D4 --> (7)F4 (583 nm), and (5)D4 --> (7)F3 (622 nm). The Na0.95Li2PO4:0.05Tb(3+) phosphor showed the most excellent emission efficiency. The present work suggests that the Na0.95Li2PO4:0.05Tb(3+) is a potential green-emitting phosphor for near ultraviolet excited light emitting diodes.