A series of stable glycine/palygorskite (GLY/PAL) nanohybrid absorbents were prepared by incorporating GLY molecules into PAL via a simple high-pressure homogenization. The structural characterization demonstrated that 3.15% of GLY molecules were incorporated into the GLY/PAL hybrid adsorbent and formed H-bonding interactions with siloxane and inner channels of PAL, which caused slight distortion of the crystalline framework. Compared with conventional surface modification, high-pressure homogenization and heat treatment enabled GLY to insert into PAL channels well to form hybrid nanostructure. Among all hybrid absorbents, the 60GLY/PAL showed the highest adsorption capacities of 147 mg/g for methyl violet (MV) and 80 mg/g for Cs(I) as well as the removal ratios of 98% for MV and 80% for Cs(I) from 150 mg/L of MV and 100 mg/L of Cs(I) solutions, respectively. In contrast, raw PAL (without modification) could adsorb only 112 mg/g of MV and 45 mg/g of Cs(I). This work has demonstrated that utilizing a simple high-pressure homogenization process improved stability of GLY/PAL nanohybrid absorbents by increasing the incorporation of guest (GLY) molecules into the tunnels/channels of hosts (PAL), leading to a novel enhanced adsorbent for Cs(I) and MV. This finding has provided a new way to fabricate nanohybrid adsorbents.