The data presented correspond to the results reported in the publication “Digital and Experimental Design of CO₂-Responsive Polymers Based on Acrylamide Monomers for Carbon Capture.”, which investigates the CO₂ capture performance of the digital and experimental designed CO₂-responsive homopolymer poly(N-[3-(dimethylamino)propyl]acrylamide) (PDMAPAm) and its diblock copolymer poly(N-[3-(dimethylamino)propyl]acrylamide)-b-poly(methyl methacrylate) (PDMAPAm-b-PMMA), with a particular focus on their integration into membrane adsorbers for direct air capture (DAC) applications. The dataset contains: 1. CO₂ adsorption-desorption isotherm of homopolymers (PDMAPAm and PMMA) with different molas masses and diblock copolymer (PDMAPAm-b-PMMA). (Data name: Data of CO₂ adsorption-desorption in dry conditions from gravimetric measurement.xlsx) 2. Change of kinetic parameters (qmax and kL) of Langmuir model with molar mass of homopolymer (PDMAPAm), PDMAPAm block content of diblock copolymer and temperature. (Data name: Data of Langmuir parameters qmax and kL.xlsx) 3. CO₂ Adsorption-desorption cycling experiments on PDMAPAm232 and on PDMAPAm232-b-PMMA57 at 1 bar and 30 °C. (Data name: Data for cycling experiments.xlsx) 4. Glass transition temperature (Tg) change of CO₂- and N₂-exposed PDMAPAm with two different molar masses at different pressures. (Data name: Data of glass transition temperature of CO2- and N2-exposed PDMAPAm.xlsx) 5. Unified model data combining polymerization kinetics with CO₂ adsorption kinetics under dry conditions. The model predicts the optimal synthesis recipe for PDMAPAm, including monomer (DMAPAm) conversion, number-average molar mass, and livingness as a function of polymerization time using the polymerization kinetic model (PDMAPAm163). Additionally, it forecasts the CO₂ adsorption capacity of the diblock copolymer PDMAPAm163-b-PMMA30 using the adsorption kinetic model. (Data name: Data of unified model.xlsx)