As the typical material of two-dimensional transition metal dichalcogenides (TMDs), few-layered MoS2 possesses broadband saturable absorption and a large nonlinear refractive index, which could be regarded as a promising candidate for dual-function photonic device fabrication. In this work, the coexistence of a bound soliton and harmonic mode-locking soliton was demonstrated in an ultrafast fiber laser based on a MoS2-deposited microfiber photonic device. Through a band-pass filter, each multi-soliton state was investigated separately. The bound soliton has periodic spectral modulation of 1.55 nm with a corresponding pulse separation of 5.16 ps. The harmonic mode-locking soliton has the repetition rate of 479 MHz, corresponding to the 65th harmonic of the fundamental repetition rate. The results indicated that there exist more possibilities of different multi-soliton composites, which would enhance our understanding of multi-soliton dynamics.