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Grinding assisted, simple and green route for the synthesis of bis(pyrazol‐5‐ole) and pyrazolopyranopyrimidine using chitosan as a biodegradable catalyst is developed. This protocol offers selective synthesis of bis(pyrazol‐5‐ole) and pyrazolopyranopyrimidine without any side product with excellent yield and shorter duration. Moreover, this method provides metal‐free synthesis and put forward easy separation in gram scale synthesis which makes the protocol sustainable. The recyclability of the catalyst is also simple and carried upto eight consecutive runs. In addition, SEM images and powder XRD of fresh and recycled catalysts are also compared.