Conventional immunochromatography (ICA) using a single-signal output mode suffers from poor sensitivity, narrow detection range, and susceptibility to external interference. The rational development of multifunctional tags is a promising strategy for integrated multimodal ICA. Herein, this study reports on multimodal ICA using "all-in-one" 2D multifunctional polygonal nanoparticles (CPPs). The spectral absorption capacity of CPPs and excellent photothermal properties (η = 89.9%) ensure the high sensitivity of ICA. The good catalytic ability enables ICA to guarantee high sensitivity while taking into account a wide detection range (expanded by about 1.5 times). Based on spectral overlap, fluorescence calibration is performed in low background to improve the practicability of ICA. The detection range of the multimodal CPPs-ICA for vomitoxin (DON) is 0.01–60 ng/mL, with the lowest qualitative and quantitative results of 0.5 and 0.021 ng/mL, respectively. This multimodal CPPs-ICA platform is expected to be an instant detection platform for multifunctional application scenarios.