Long persistent luminescence (LPL) materials with color adjustable afterglow have a wide application prospect in display and information encryption, yet there are few reports on such materials. In this paper, SrZn2(PO4)2 phosphors with tunable and thermal stimuli-responsive afterglow emissions were synthesized by a solid-state method. After ultraviolet (UV) excitation, the prepared samples exhibited emission at 419 nm, 533 nm, and 633 nm due to Eu2+: 4f65d1 → 4f7 transitions, Mn2+: 4T2(4G) →6A1(6S) transitions, and Mn2+: 4T1(4G) → 6A1(6S) transitions, respectively. The Commission Internationale de I’ Eclairage (CIE) coordinates of samples can be changed among blue, white, and yellow by varying the Mn2+ concentration. Additionally, due to the differing thermal stability of Eu2+ and Mn2+, the phosphor exhibited a temperature-responsive afterglow, and its colors can be adjusted between white and yellow over a temperature range from 293 K to 383 K. Given its distinctive temperature-responsive afterglow, the prepared phosphor is suitable for use as a temperature sensor. Moreover, the tunable afterglow colors of the phosphors are advantageous for application in anti-counterfeiting.