The accumulation of original phosphogypsum (OPG) has occupied considerable land resources, which have induced significant environmental problems worldwide. The OPG-based cemented paste backfill (OCPB) has been introduced as a promising solution. In this study, a water-washing pre-treatment was used to purify OPG, aiming to optimize the transport performance and mechanical properties of backfills. The overall results proved that in treated phosphogypsum-based cemented paste backfill (TCPB), the altered particle size distribution can alleviate the shear-thinning characteristic. The mechanical properties were significantly optimized, of which a maximum increase of 183% of stress value was observed. With more pronounced AE signals, the TCPB samples demonstrated better residual structures after the ultimate strength values but with more unstable cracks with high amplitude generated during loading. Principal component analysis confirmed the adverse effects of fluorine and phosphorus on the damage fractal dimensions. The most voluminous hydration products observed were amorphous CSH and ettringite. The interlocked stellate clusters may be associated with the residual structure and the after-peak AE events evident in TCPB, indicate that more significant stress should be applied to break the closely interlocked stitches. Ultimately, the essential findings in this experimental work can provide a scientific reference for efficient OPG recycling.