Effective separation and transfer of photoexcited carriers are essential for photocatalysis, which could be optimized by the rational design of morphology and phase structure. Herein, using NH 4 HCO 3 as intercalating and orienting agents, few-layer vertical-standing multiphasic MoS 2 nanosheets (VM-MoS 2 ) were successfully constructed along the longitudinal axis of CdS nanorods via a green hydrothermal method. The growth mechanism of VM-MoS 2 on CdS nanorods was demonstrated to include the competitive adsorption of HCO 3 − and Mo 7 O 24 6− anions on the protonated CdS, and the intercalation of NH 4 + cations. Moreover, the impacts of the morphology and phase structure of the MoS 2 cocatalyst on the photocatalytic H 2 evolution (PHE) performance of CdS were carefully compared. It is found that the VM-MoS 2 nanosheets can not only expose abundant active sites, but also allow the supporter to harvest the light effectively. Additionally, the metallic 1T-MoS 2 in VM-MoS 2 would help the interface transfer of photogenerated electrons and act as photoelectron entrepots and catalytically active sites for H 2 evolution. With the VM-MoS 2 cocatalyst, the as-synthesized CdS@ VM-MoS 2 shows an outstanding PHE rate of ∼40.1 mmol•h −1 •g −1 under visible-light irradiation. Interestingly, integrating with the 2H-MoS 2 phase will make the metastable 1T-MoS 2 more stable, leading to the exceptional photostability of CdS@VM-MoS 2 nanocomposite.