Replicating the functions and movements of biological systems is an enduring goal of soft robotics, which use compliant materials to mimic soft bodied organisms. The development of new materials and advanced fabrication methods is critical to continue to expand the field of soft robotics. Soft composites pose a promising solution for recreating the properties and actuation of natural beings. Precise control of the mechanical, electrical, and chemical properties of these composites is made possible by modulating their constituent materials. A wide range of methods have been developed for fabricating these soft composites; however, of these techniques, photopolymer additive manufacturing (AM) has been shown to offer unrivaled speed as well as control of composition, geometry, function, and complexity. In recent years, Computed Axial Lithography (CAL), a volumetric AM approach, has been shown to be ideal for creating smooth surfaces with high resolution and unparalleled speed. Overprinting, a practically unexplored process made possible with CAL, also offers exciting potential applications. This work makes three contributions to the field of photopolymerizable soft composite materials and fabrication methods. First, a method for scaling up CAL is proposed which uses active cooling to counteract heat generation and enabling the manufacture of the largest CAL print to date (70.2 cm^3) in just minutes. This also represents a throughput over 5 times that of previous reported values (23.4 cm^3/min^(-1)). This large-scale CAL printing was made possible with the use of a 4k light engine incorporated into a custom-built CAL printer. Next, an overprinted hydrogel osmotic actuator is printed with directed bending actuation of up to 60° demonstrating the first functional overprint. A ray-based dose calculation method is also described which allows for print-time prediction for overprinting. And finally, a soft and tough composite is developed by combining collagen with a zwitterionic hydrogel. This work highlights a simple synthesis method, biocompatibility (>90% cell viability), and elastic modulus (E= 0.180 MJ) and toughness (W^*= 0.617 MJ m-3) approaching that of biological tissues such as articular cartilage. Most notably, the addition of only 15 mg mL^(-1) collagen to this network increases the fracture toughness nearly 11-fold (Γ= 180 J m-2).