Partially neutralized acrylic acid (AA)/sodium acrylate (NaAA) and N, N′‐methylenebisacrylamide (MBA) were subjected to intercalative copolymerization in aqueous solution of polyvinyl alcohol (PVA) in the presence of sodium montmorillonite (NaMMT) nano clay to prepare filled semi‐interpenetrating network (FSIPN) type composite polymer networks. Filled Full IPN (FFIPN) composites were prepared in a similar way by additional crosslinking of PVA with maleic acid (MA) crosslinker. The polymers were characterized with FTIR, NMR, XRD, TGA, SEM, EDAX, TEM, XPS, DLS, PZC, and pH reversibility test. The synthesis variables were optimized with respect to batch adsorption of 100 mg/L each of methyl violet (MV) and congo red (CR) dye as response using the central composite design (CCD) of response surface methodology (RSM). The FFIPN prepared from polyacrylic acid (PAA)/sodium polyacrylate containing PVA/Clay/MBA/MA of optimized composition of 4/1.5/0.75/4 (wt.% of AA/NaAA), respectively, showed an optimized adsorption (mg/g adsorbent) of 459.16/417.31 of MV/CR as single dye and 438.01/417.31 of MV/CR in 1:1 binary mixtures of 100 mg/L feed concentration. The FFIPN showed an adsorption (mg/g) of 41.54/37.61 and removal% of 88.5/80.12 at a feed flow rate, bed height, and feed inlet concentration of 20 mL/min, 20 mm, and 50 mg/L, respectively.