A green and in-situ metal-organic framework (MOF) shaping strategy was proposed to fabricate cellulose foam HKUST-1 and modify with polysaccharides for convenient adsorption applications. The obtained unique foam HKUST-1 not only maintains HKUST-1 intrinsic thermal stability and high surface area, but also exhibits unique crystal structure and interface for HKUST-1. Moreover, the surface and crystal size of foam HKUST-1s can be easily modulated with natural polysaccharides, and the crystal and novel interfaces awarded them 5.2 times higher adsorption uptake (4.52 mmol/g) for vapor-toluene than MIL-101 (Cr) under low pressure P/Po approximate to 0.0026 and high selectivity (1 0 7) for acidic/basic dipeptides EE/RR. Based on the above results, the novel foamed MOFs can be applied for volatile organic compounds (VOCs) adsorption under ambient condition and improve acidic dipeptides enrichment in liquid phase. It will play a significant role as adsorbent in practical adsorption applications.