Solid acids have been proposed as a hydrolytic agent for wood biomass dissolution. In this work, we presented an environmentally friendly physicochemical treatment to leave behind cellulose, dissolve hemicellulose, and remove lignin from poplar wood. Several pretreatments, such as autohydrolysis and disk refining, were compared to optimize and modify the process. The p-toluenesulfonic acid could extract lignin from wood with a small amount of cellulose degradation. Disk refining with subsequent acid hydrolysis (so-called physicochemical treatment) doubled the delignification efficiency. A comprehensive morphology and overall chemical composition were provided. The crystallinity index (CrI) of treated poplar was increased and the chemical structure was changed after physicochemical treatment. Optical microscopy and scanning electron microscopy analysis demonstrated physicochemical treatment affected the morphology of poplar wood by removing lignin and generating fiberization. In general, this work demonstrated this physicochemical method could be a promising fractionation technology for lignocellulosic biomass due to its advantages, such as good selectivity, in removing lignin while preserving cellulose.