This book presents a wide panorama of methods to investigate the spectral properties of block operator matrices. Particular emphasis is placed on classes of block operator matrices to which standard operator theoretical methods do not readily apply: non-self-adjoint block operator matrices, block operator matrices with unbounded entries, non-semibounded block operator matrices, and classes of block operator matrices arising in mathematical physics.The main topics include: localization of the spectrum by means of new concepts of numerical range; investigation of the essential spectrum; variational principles and eigenvalue estimates; block diagonalization and invariant subspaces; solutions of algebraic Riccati equations; applications to spectral problems from magnetohydrodynamics, fluid mechanics, and quantum mechanics.