Mountain pine beetle-killed lodgepole pine (Pinus contorta) chips were pretreated using the organosolv process, and their ease of subsequent enzymatic hydrolysis was assessed. The effect of varying pretreatment chemicals and solvents on the substrate's physicochemical characteristics was also investigated. The chemicals employed were MgCl2, H2SO4, SO2, and NaOH, and the solvents were ethanol and butanol. It was apparent that the different pretreatments resulted in variations in both the chemical composition of the solid and liquid fractions as well in the extent of cellulolytic hydrolysis (ranging from 21% to 82% hydrolysis after 12 h). Pretreatment under acidic conditions resulted in substrates that were readily hydrolyzed despite the apparent contradiction that pretreatment under alkaline conditions resulted in increased delignification (approximately 7% and 10% residual lignin for alkaline conditions versus 17% to 19% for acidic conditions). Acidic pretreatments also resulted in lower cellulose degree of polymerization, shorter fiber lengths, and increased substrate porosity. The substrates generated when butanol/water mixtures were used as the pretreatment solvent were also hydrolyzed more readily than those generated with ethanol/water. This was likely due to the limited miscibility of the solvents resulting in an increased concentration of pretreatment chemicals in the aqueous layer and thus a higher pretreatment severity.