Due to the dramatically increasing production of excess sludge during biological wastewater treatment, the development of an economical, efficient, and environmentally friendly sludge dewatering method is highly required. Herein, Bdellovibrio-and-like organisms (BALOs), a group of predatory bacteria were applied for waste sludge dewaterability enhancement and biomass reduction and the potential biolysis mechanisms were elaborated. Generally, the satisfying biolysis performance was obtained for the sludge with the moderate total solid (TS) content (1.5–2.5%). Within 24-h sludge biolysis with our isolated and enriched BALOs, the sludge specific resistance to filtration value as the dewaterbility index reached the maximal reduction rate of 65.3 ± 6.4%. Meanwhile, the concentrations of released soluble nitrogen and phosphorous significantly increased by 57.4 ± 3.3 and 56.7 ± 6.1%, respectively. Moreover, the contents of tightly bound extracellular polymeric substances (EPS) dramatically decreased after sludge biolysis while the loosely bound EPS contents increased, which implied the disruptions of sludge flocs structure for sludge dewaterability improvement. High-throughput sequencing results revealed the remarkable shift of sludge’s microbial community structure after biolysis treatment. The relative abundances of the dominant genera Ferruginibacter, Pseudomonas, and Thermomonas related to denitrification or flocs structure stabilization dramatically decreased. The noticeable increasing populations of Comamonas and Hyphomicrobium in abundances suggested the potential re-growth of the surviving microbial cells in response to BALO invasions. Overall, BALO predation could disintegrate the waste sludge structure, promote the cell lysis and the intracellular substances release, and cause the variations of microbial community compositions to efficiently improve the sludge dewaterability.