A fluorometric and colorimetric dual-modal nanoprobe (denoted as Fe-Phen/SiNPs) has been developed for selective and sensitive determination of nitrite (NO). The mechanism is based on fluorescence quenching between silicon nanoparticles (SiNPs) and Fe(II)-phenanthroline complex (Fe-Phen) via inner filter effect and redox. With the addition of increasing NO, Fe is oxidized to Fe, recovering the fluorescence of SiNPs. Meanwhile, the color of the system gradually changes from orange-red to colorless, which enables colorimetric measurement. The NO concentration shows a wide linear relationship with fluorescence intensity from 0.1 to 1.0 mM (R = 0.9955) with a detection limit of 2.4 μM in the fluorometric method (excitation wavelength: 380 nm). By contrast, the linear range of the colorimetric method ranges from 0.01 to 0.35 mM (R = 0.9953) with a limit of detection of 6.8 μM (proposed selective absorbance: 510 nm). The probe has been successfully applied to nitrite determination in water, salted vegetables, and hams demonstrating broad application prospects for the determination of nitrite in complicated matrices.