Carrageenan fibers crosslinked with trivalent metal ions (Al3+ or Fe3+) were prepared into carrageenan fiber paper (Al/CAP, Fe/CAP) by the Rapid Kothen method, and their flame-retardant mechanism and flame retardancy were studied through LOI, VF, SEM, CONE, and TGA testing. The results showed that Al/CAP exhibited good flame retardancy and thermal stability, and its LOI value reached 52%. Meanwhile, the afterflame time and afterglow time of Al/CAP were 0 and 1 s, respectively, which indicated that it was not ignited and almost had no smoldering phenomenon. The flame-retardant performance of Fe/CAP is inferior to that of Al/CAP, with LOI of 32, but the total smoke emission (TSP) of Fe/CAP is lower in cone calorimetry test. Thus, CAPs (especially Al/CAP) can be widely used in the flame-retardant paper industry, due to their flame retardancy and environmental protection.