MoS 2 nanomaterial with the micro-pompon structure was synthesized by a surfactant-assisted hydrothermal method. The morphologies and structures of as-prepared MoS 2 micro-pompon were investigated by adding different types of surfactants such as cetyltrimethyl ammonium bromide (CTAB), sodium dodecylbenzene sulphonate (SDBS), and polyvinyl pyrrolidone (PVP). The results indicated that the morphology of MoS 2 could be controlled and changed effectively by the cationic surfactant of CTAB. A reasonable growth mechanism for hollow structured MoS 2 micro-pompon by hydrothermal processes was proposed. Further, photocatalytic degradation properties of MoS 2 micro-pompon under visible light were evaluated by degradation of common organic dyes, which include rhodamine B (RhB), congo red, methyl orange, and methylene blue. The results indicated that MoS 2 micro-pompon owned the highly selective catalytic ability to RhB with degradation efficiency of 95% in 60 min and 68% in 30 min. With the additive of the surfactant, the MoS 2-CTAB sample exhibited an enhanced ability of photocatalytic activity where degradation efficiency was improved to 92% in 30 min. The method employed in this work could be expanded to fabricate other sulfides with the controllable morphology and structure to further regulate the photocatalytic performance.