This doctoral thesis by Juan Luis Jerez focuses on developing more efficient computational methods and custom hardware architectures for real-time optimal decision making and control applications. The thesis proposes techniques to exploit synergies between digital hardware, numerical algorithms, and algorithm design. These include custom storage schemes, parallel optimization approaches, tailored linear algebra methods for fixed-point arithmetic, and finite-precision analysis of first-order optimization methods. The techniques are demonstrated on examples such as a hardware-in-the-loop setup for model predictive control of a large airliner.