High‐entropy alloys (HEAs) possess superior mechanical, thermal, and electronic properties, which attract great interest in the fields of photothermal, electrocatalysis, and magnetic applications. Herein, the nonlinear optical properties of FeCoNiAlTi HEA with a large specific surface area for the first time is investigated. Owing to the strong d–d interaction, the interband transition near the Fermi level could be enhanced in HEAs, leading to broadband optical absorption. Excitation with the picosecond laser source, the FeCoNiAlTi HEA possesses saturable absorption with a large modulation depth of 7.61% and 30.47% at 1 and 1.5 µm, respectively. Furthermore, at the higher excitation level at 1.5 µm, the saturable absorber exhibits a typical reverse saturable absorption property. Subsequently, the FeCoNiAlTi HEA on the tapered fiber first serves as the saturable absorber in the Yb‐doped fiber laser and the Er‐doped fiber laser, leading to the noise‐like pulses at 1 µm, and the stable Q‐switching, conventional soliton, and dissipative soliton resonance mode‐locking operations at 1.5 µm. This work confirms that the enhanced saturable absorption in HEAs can endow the high‐performance ultrashort pulse generation.