Bamboo is a material with excellent development prospects. It is increasingly used in furniture, decoration, building, and bridge construction. In this study, Furfurylated bamboo bundles and phenol-formaldehyde resin were used to make bamboo-scrimber composites (BSCs) via molding-recombination and hot-pressing processes. The effects of the impregnation mode, furfuryl-alcohol concentration, and curing temperature on the various physical–mechanical properties and durability of the composites were evaluated. Scanning-electron microscopy (SEM) was used to observe the microstructural differences. Fourier-transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS) were employed to investigate changes in the chemical constituents. The heat resistance was also investigated using thermogravimetric analysis. The results showed that the density of the furfurylated BSC increased by up to 22% compared with that of the BSC-C with the same paving mode. The furfurylated BSCs had lower moisture contents: the average moisture content of the furfurylated BSCs was 25~50% lower than that of the BSC-C. In addition, the furfurylated BSCs showed better dimensional stability and durability, since the decay-resistance grade of the BSCs was raised from decay resistance (class II) to strong decay resistance (class I). In terms of the mechanical properties, the furfurylation had a slight negative effect on the mechanical strength of the BSCs, and the modulus of rupture (MOR) and horizontal shear strength (HSS) of the BSCs were increased to a certain extent under most of the treatment conditions. In particular, the highest HSS for indoor use and MOR of the furfurylated BSCs increased by 21% and 9% compared with those of the untreated BSCs, respectively. The SEM results indicated that the FA resin effectively filled in the bamboo-cell cavities and vessels, and the modified bamboo-parenchyma cells were compressed more tightly and evenly. The FTIR and XPS spectroscopy showed that the hydroxyl group of carboxylic acid of the bamboo-cell-wall component reacted with that of the furan ring, and the cellulose and hemicellulose underwent acid hydrolysis to a certain extent after the furfurylation. Overall, the present study highlights the potential of furfurylation as a modification method to enhance BSC products. Further research should focus on improving the ability of furfurylated BSCs to prevent the growth of Botryodiplodia theobromae. Additionally, the influence of furfuryl-alcohol resin on the bonding strengths of PF adhesives should be further clarified.