Highly typical tetra-substituted pyrroles 4a-j were prepared by the condensation of 1,3-dicarbonyl compounds, benzoin, and ammonium acetate via a one-pot hydrothermal synthesis procedure in the presence of sulfamic acid (SA), as a solid-phase organic catalyst which has recently become quite popular. The efficiency of SA as a new catalyst and ZnCl2 as traditional catalyst in the synthesis of 1-(2-methyl-4,5-diphenyl-1H-pyrrol-3-yl)ethanone 4a was performed as an example for the present comparison. Scanning electron microscopy (SEM) was used to compare the morphologies of the 1-(2-methyl-4,5-diphenyl-1H-pyrrol-3-yl)ethanone films 4a that prepared by those catalysts. An appropriate ratio of sulfamic acid was enough to start the reaction with a higher yield and a higher surface area to volume ratio. Besides, it provided nanoscale-interpenetrating networks with homogenous structures. The chemical structure of the target compounds was characterized by NMR and FTIR spectroscopy. In addition, the prepared compounds were evaluated to study their antimicrobial and antioxidant activities.