This study demonstrated the potential of simultaneously recovering cellulosic solid residues (CSR) and producing cellulose nanocrystals (CNCs) by strong sulfuric acid hydrolysis to minimize cellulose loss to near zero. A set of slightly milder acid hydrolysis conditions than that considered as “optimal” were used to significantly minimize the degradation of cellulose into soluble sugars that cannot be economically recovered, but resulted in CSR that is easily recoverable through conventional centrifuge. It was found that the window for simultaneous recoveries of CSR and producing high yield CNC in strong acid hydrolysis was extremely narrow. However, we achieved significant CSR yield with near zero cellulose loss but without sacrificing CNC yield compared with that obtained at “optimal condition”. The resultant CSR contains sulfate ester groups that facilitated subsequent mechanical nano-fibrillation to cellulose nanofibrils (CNFs), a potential high value nanocellulosic material for a variety of applications.