The interaction of DNA with the polymeric nano and microcarriers has been attracted significant attention in the studies on DNA diagnostic assays, DNA isolation, particularly gene delivery and cancer therapy agents. Therefore, in this study, plain poly(glycerol dimethacrylate) and poly(dimethylaminoethyl methacrylate) grafted-poly(glycerol dimethacrylate) microgel particles were synthesized for high single-stranded DNA (ssDNA) adsorption and desorption capacity. Temperature and pH-sensitive uniform poly(GDMA) particles were synthesized through a two-stage procedure. GDMA (glycerol dimethacrylate) dispersion polymerization procedure was used in the first stage of the study to get microgel particles approximately 900 nm in size. Surface-initiated ATRP (Atom Transfer Radical Polymerization) procedure, a living polymerization technique of 2-dimethylaminoethyl methacrylate (DMAEM), was used in the second stage of the study to get polycationic molecular brushes on microgel particles. The resulting temperature and pH-responsive microgel were used as sorbent for ssDNA adsorption. As compared to commonly used sorbents, reasonably high ssDNA adsorptions were achieved with the proposed sorbent. The adsorbed ssDNA was desorbed from the sorbent with high yield. The adsorption and desorption behaviors make poly(DMAEM) grafted-poly(GDMA) microgel particles as a promising carrier/sorbent for ssDNA.