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In this study, we evaluated the pelleting characteristics of southern yellow pine (SYP), switchgrass (SG), and their blends for thermochemical conversion processes, such as pyrolysis and gasification. Using a pilot-scale ring-die pellet mill, we specifically assessed the impact of blend moisture, length-to-diameter (L/D) ratio in the pellet die, and ratio of pine to SG on the physico-chemical properties of the resulting pellets. We found that an increase in pine content by 25–50% marginally affected the bulk density; however, it also led to an increase in calorific value by 7% and a decrease in ash content by 72%. A moisture content of 25% (wet basis) and an L/D ratio of 5 resulted in poor pellet durability at 90% and the bulk density to >500 kg/m3. Blends with ≥50% pine content resulted in lower energy consumption, while a lower L/D ratio resulted in higher pelleting energy. Based on these findings, we successfully demonstrated the high-moisture pelleting of 2.5 ton of pine top residues blended with SG at 60:40 and 50:50 ratios. The quality of the pellets was monitored off-line and at-line by near infrared (NIR) spectroscopy. Multivariate models constructed by combining the NIR data and the pelleting process variables could successfully predict the pine content (R2 = 0.99), higher heating value (R2 = 0.98), ash (R2 = 0.95), durability (R2 = 0.94), and bulk density (R2 = 0.86) of the pellets. Thus, we established how blending and densification of SYP and SG biomass could improve feedstock specifications and that NIR spectroscopy can effectively monitor the pellet properties during the high-moisture pelleting process.