Metal–organic frameworks (MOFs) improved several trends and are promising for industrial applications. However, current synthesis processes offer powder form, rendering their applications difficult. A simple solvothermal method offered an in situ growth of copper-based MOFs, for example, CuBDC (BDC: benzene-1,4-dicarboxylic acid) into a cotton textile; the material was denoted as CuBDC@Textile. CuBDCTextile was used as a solid sensor and adsorbent for volatile organic compounds (VOCs). It exhibited good vapochromic properties that enabled a colorimetric detection of pyridine (Py) via naked eyes with high selectivity and good sensitivity. Adsorption of pyridine via pervaporation using CuBDC@Textile was recorded. CuBDCTextile is a flexible textile with a high adsorption capacity (137.9 mg g⁻¹) toward pyridine. It offered dual functional: sensor probe and adsorbent. The synthesis of CuBDC@Textile and their excellent performance as a sensor and adsorbent are promising for further investigation of the “MOFs on textile materials” topic.