Radioactive strontium (90Sr) is considered as one of the most dangerous radionuclides due to its high biochemical toxicity. For the efficient and selective separation of Sr from acidic environments, a novel functional adsorbent CEPA@SBA-15-APTES was prepared in this work through the phosphorylation of amino-modified mesoporous silica with organic content of approximately 20 wt%. CEPA@SBA-15-APTES was characterized by TEM, SEM, EDS, TG-DSC, BET, FTIR, and XPS techniques, revealing its characteristics of an ordered hexagonal lattice-like structure and rich functional groups. The experimental results demonstrated that the adsorbent exhibited good adsorption capacity for Sr over a wide acidity range (i.e., from 10−10 M to 4 M HNO3). The adsorption equilibriums of Sr by CEPA@SBA-15-APTES in 10−6 M and 3 M HNO3 solutions were reached within 30 and 5 min, respectively, and the adsorption capacities at 318 K were 112.6 and 71.8 mg/g, respectively. Furthermore, by combining the experimental and characterization results, we found that the adsorption mechanism consisted of ion exchange between Sr(II) and H+ (in P-OH) in the 10−6 M HNO3 solution and coordination between the Sr(II) and oxygen-containing (CO and P = O) functional groups in the 3 M HNO3 solution.