Molybdate sulfuric acid (MSA) and silica sulfuric acid (SSA) has been prepared and used as efficient solid catalysts for the synthesis of gem-bisamides and bisurides via the one-pot three-component reaction of two moles of amides, nitriles, carbamates or urea with aldehydes. The catalytic efficiency of SSA, MSA, or H2SO4 98% per H+ sites as turnover number (TON), turnover frequency (TOF), and atomic economy (AE) was calculated and compared for quantitative evaluation of catalysts. The AE, TON, and TOF factors show the superiority of the SSA versus MSA and H2SO4. Short reaction times, simple work-up, chemoselectivity, low loading, and reusability of solid acid catalysts are extra advantages than current methods reported in the literature with corrosive acidic catalysts. (C) 2012 Elsevier B.V. All rights reserved.