Photocatalysis currently faces a number of challenging issues, such as low efficiency, expensive precursors of noble metals, and difficult recycling of powder, which are grievous impeders for powder photocatalysts in practical applications of environmental remediation. Hence, we have fabricated desirable cabbagelike floating Bi-Bi2S3-Bi2WO6@EP (expanded perlite) photocatalysts via a one-pot modified hydrothermal process. The structural morphology and reaction mechanism of as-fabricated designed photocatalysts were comprehensively investigated by physicochemical techniques. The photocatalytic efficacies of 1% Bi-Bi2S3-Bi2WO6@EP were obviously evaluated by the degradation of 4-chlorophenol (4-CP), rhodamine B (RhB), and methyl orange (MO) with enhanced rate constants (k) of 0.051, 0.073, and 0.075 min(-1), respectively, utilizing nunlike irradiation. All these enhanced photocatalytic efficacies are assigned to the successful deposition of optimal contents of ternary heterojunction (3C), surface plasmon resonance effect (SPR) of Bi, enhanced photocurrent, maximum mobility of photoinduced charge carriers, efficient direct illumination, and aerated oxygenation and photogeneration of most reactive species.