Matrix Approximation for Large-scale Learning Modern learning problems in computer vision, natural language processing, computational biology, and other areas are often based on large data sets of thousands to millions of training instances. However, several standard learning algorithms, such as kernel-based algorithms, e.g., Support Vector Machines, Kernel Ridge Regression, Kernel PCA, do not easily scale to such orders of magnitude. This thesis focuses on sampling-based matrix approximation techniques that help scale kernel-based algorithms to large-scale datasets. We address several fundamental theoretical and empirical questions including: What approximation should be used? We discuss two common sampling-based methods, providing novel theoretical insights regarding their suitability for various applications and experimental results motivated by this theory. Our results show that one of these methods, the Nystrom method, is superior in the context of large-scale learning. Do these approximations work in practice? We show the effectiveness of approximation techniques on a variety of problems. In the largest study to-date for manifold learning, we use the Nystrom method to extract low-dimensional structure from high-dimensional data to effectively cluster face images. We also report good empirical results for kernel ridge regression and kernel logistic regression. How should we sample columns? A key aspect of sampling-based algorithms is the distribution according to which columns are sampled. We study both fixed and adaptive sampling schemes as well as a promising ensemble technique that can be easily parallelized and generates superior approximations, both in theory and in practice. How well do these approximations work in theory? We provide theoretical analyses of the Nystrom method to understand when this technique should be used. We present guarantees on approximation accuracy based on various matrix properties and analyze the effect of matrix approximation on actual kernel-based algorithms. This work has important consequences for the machine learning community since it extends to large-scale applications the benefits of kernel-based algorithms. The crucial aspect of this research, involving low-rank matrix approximation, is of independent interest within the field of numerical linear algebra.