Adsorption has been used widely to remove indoor volatile organic compounds (VOCs). However, the large diffusion resistance inside traditional granular adsorbents renders a low VOC adsorption rate. This study proposes a modified method to achieve the rapid diffusion into the adsorbent during the initial adsorption period. A thin and flexible adsorption board with a layer of adsorbent coated on a heating film was prepared for in-situ adsorption and regeneration. Then, regular, vertical macro-channels through the adsorption board were fabricated by laser drilling to enhance mass transfer inside the board. Experimental results demonstrated that after modification, the penetration times for formaldehyde and xylene extended from 3.8 to 6.2 h, and from 62 to 99 h, respectively. The effective adsorption capacity of the modified board had increased by a multiple of two for formaldehyde and 1.8 for xylene. A mathematical model was developed and experimentally validated to evaluate the modification effect for more adsorbent-pollutant pairs. The results showed that the amplification of effective adsorption capacity was positively correlated with the Da/(K·De) parameter; this is the diffusion resistance ratio prior to and following the modification. A spectrogram of adsorbent–pollutant pairs was plotted to guide the modification. This simple macro-channel modification of the adsorption board may be used as an alternative design for adsorption applications in indoor air purification.