This paper focuses on the preparation and evaluation of a novel humidity-control material, vermiculite/(sodium polyacrylate(AA)–acrylamide(AM)), using inverse suspension polymerization. Acrylic acid and acrylamide were introduced into the interlayer of modified vermiculite during the polymerization process, leading to the formation of a strong association with the modified vermiculite. The addition of vermiculite increased the specific surface area and pore volume of the composites. To investigate the moisture absorption and desorption properties of the composites, an orthogonal experiment and single-factor experiment were conducted to analyze the impacts of vermiculite content, neutralization degree, and the mass ratio of AA to AM. According to the control experiment, the addition of vermiculite was found to enhance the pore structure and surface morphology of the composite material, surpassing both vermiculite and PAA-AM copolymer in terms of humidity control capacity and rate. The optimal preparation conditions were identified as follows: vermiculite mass fraction of 4 wt%, a neutralization degree of 90%, and mAA:mAM = 4:1. The moisture absorption rate and moisture release rate of the composite material prepared under these conditions are 1.285 g/g and 1.172 g/g. The humidity control process of the composite material is governed by pseudo second-order kinetics, which encompasses the complete adsorption process. These results indicate that the vermiculite/PAA-AM composite humidity control material has excellent humidity control performance and is a simple and efficient humidity control method.