Complementary Metal-Oxide-Semiconductor (CMOS) technology is currently the most widely used integrated circuit technology today. As CMOS approaches the physical limitations of scaling, it is unclear whether or not it can provide long-term support for niche areas such as high-performance computing and telecommunication infrastructure, particularly with the emergence of cloud computing. Alternatively, superconductor technologies based on Josephson junction (JJ) switching elements such as Rapid Single Flux Quantum (RSFQ) logic and especially its new variant, Energy-Efficient Rapid Single Flux Quantum (ERSFQ) logic have the capability to provide an ultra-high-speed, low power platform for digital systems. The objective of this research is to design and evaluate energy-efficient, high-speed 32-bit integer Arithmetic Logic Units (ALUs) implemented using RSFQ and ERSFQ logic as the first steps towards achieving practical Very-Large-Scale-Integration (VLSI) complexity in digital superconductor electronics. First, a tunable VHDL superconductor cell library is created to provide a mechanism to conduct design exploration and evaluation of superconductor digital circuits from the perspectives of functionality, complexity, performance, and energy-efficiency. Second, hybrid wave-pipelining techniques developed earlier for wide datapath RSFQ designs have been used for efficient arithmetic and logic circuit implementations. To develop the core foundation of the ALU, the ripple-carry adder and the Kogge-Stone parallel prefix carry look-ahead adder are studied as representative candidates on opposite ends of the design spectrum. By combining the high-performance features of the Kogge-Stone structure and the low complexity of the ripple-carry adder, a 32-bit asynchronous wave-pipelined hybrid sparse-tree ALU has been designed and evaluated using the VHDL cell library tuned to HYPRES' gate-level characteristics. The designs and techniques from this research have been implemented using RSFQ logic and prototype chips have been fabricated. As a joint work with HYPRES, a 20 GHz 8-bit Kogge-Stone ALU consisting of 7,950 JJs total has been fabricated using a 1.5 ??m 4.5 kA/cm^2 process and fully demonstrated. An 8-bit sparse-tree ALU (8,832 JJs total) and a 16-bit sparse-tree adder (12,785 JJs total) have also been fabricated using a 1.0 ??m 10 kA/cm^2 process and demonstrated under collaboration with Yokohama National University and Nagoya University (Japan).