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The implementation of covalent adaptable networks (CANs) in general resin system is becoming attractive. In this work, we propose a simple post‐curing strategy based on the core‐shell structured acrylate latex for the achievement on both the improved general performance and the CANs characteristics in latex films. The building to the CANs was relied on the introduction of 4,4′‐diaminophenyl disulfide as the curing agent, which cured the acetoacetoxy decorated shell polymer through the ketoamine reaction. The metathesis reaction of aromatic disulfides in the crosslinking segments enabled the thermally induced dynamic behavior of the network as revealed in the stress relaxation tests by comparison with other diamine crosslinking agents without the incorporation of disulfide. The synergism of the dynamic crosslinking of the shell polymer and static crosslinking in the core polymer contributed to the improved mechanical strength (15 MPa, strain% = 250%) and the suppressed water adsorption (~1% in 24 h of soaking) of the latex film, which exhibited above 90% of recovery in both strength and strain from a cut‐off film damage within 1 h at 80°C. Moreover, the cured latex film could be recycled, and 75% of the mechanical performance was regained after three fragmentation‐hot‐pressing cycles. These, in addition with the feasible and environmental friendly characteristics, suggest a sustainable paradigm toward the smart thermosetting latex polymers.

Through a novel method, we successfully synthesized electromagnetic (EM) functional polystyrene@polypyrrole@nickel (PS@PPy@Ni) composite microspheres. The PS@PPy spheres with well-defined core/shell structure have been synthesized via an in situ chemical oxidative copolymerization of pyrrole (Py) and N-2-carboxyethylpyrrole (PyCOOH) templated by PS microspheres. The reaction was carried out under heterophase conditions using the mixture of ethanol and water as the continuous phase. Tailored by the carboxyl groups on the surface of microspheres, magnetic nickel layer has been steady deposited onto the P(Py-PyCOOH) layer of the microspheres through an activation-electroless plating technology. The fine PS@P(Py-PyCOOH)@Ni core/shell structures could be obtained with the PyCOOH content up to 50 wt % in the P(Py-PyCOOH) layer. Moreover, the as-prepared PS@P(Py-PyCOOH)@Ni composites are ferromagnetic materials and behave as a good electromagnetic (EM) absorption material due to the coating of Ni layer around the PS@P(Py-PyCOOH) spheres. The PS@P(Py-PyCOOH)@Ni composite spheres show the remarkable EM wave absorption property with the maximum reflection loss (around −20.06 dB) at 10.69 GHz. The EM wave absorption can retained lower than −10 dB within a broad frequency range from 9.16 to 13.75 GHz.