Natural-based lignocellulose fibrous materials can be used as a sustainable alternative to conventional fossil-based fibers such as glass fibers, in lightweight fiber-reinforced thermoplastic composites for marine, automotive, aerospace, or other advanced applications. However, one of the main challenges in using natural fiber-based thermoplastic composites is the low mechanical performance of composite structures. This can be improved significantly through the development of an optimized novel fiber architecture with enhanced fiber packing properties, following a low-cost production process. In this context, this study demonstrates a less energy-consuming and cheaper manufacturing process, for developing highly individualized short jute fiber-based dry fiber preform architecture, with an improved fiber packing property. Short jute fibers were chemically treated with alkali and PVA sizing treatments in the processing of new fiber preform architectures, and they were used in manufacturing of ultimate short jute fiber/polypropylene (PP) thermoplastic composites. The newly developed short fiber thermoplastic composites showed a significant improvement in mechanical properties (tensile, flexural, and impact) compared to any other natural fiber architecture-based (woven, knitted, nonwoven, unidirectional, etc.) composites found in the literature. Due to the use of new fiber architecture, the developed composites’ fiber content was observed to increase. In addition, the compatibility of jute fibers with the polypropylene matrix was strengthened with the application of chemical treatments on highly individualized jute fibers. These reasons were responsible for the enhancement of mechanical properties of developed composites. Micromechanics of the fibers in composites were evaluated using the modified rule of the mixture and Halpin–Tsai equations for stiffness prediction of the composites in order to develop a theoretical understanding of newly developed composites’ mechanics. It is thought that the improved mechanical performance of short jute fiber/PP thermoplastic composites can extend the use of these composites in many load-demanding applications, wherein normally synthetic fiber composites are used.