In this investigation, transient crosslinking was constructed to obtain a hydrogel with excellent mechanical and self-healing properties. Firstly, core–shell particles with hydrophilic amino groups were prepared by emulsion polymerization and subsequently dispersed into hydrophobic association polyacrylamide hydrogels. Transient crosslinking was constructed through hydrogen bonding between core–shell particles and polyacrylamide. As a result, the hydrogels exhibited a tensile strength of 1.4 MPa and self-healing efficiency of 98% at 24 h. Furthermore, reconstruction of the transient crosslinking was confirmed from rheological measurements. Therefore, the essential reinforcement principle based on transient crosslinking would open a novel strategy to obtain hydrogels with superior toughness and self-healing properties.