This is a first paper in a series of two. In both papers, we consider the question of control of Maxwell's equations in a homogeneous medium with positive conductivity by means of boundary surface currents. The domain under consideration is a cube, where the conductivity is allowed to take on any nonnegative value. An additional restriction imposed in order to make this problem more suitable for practical implementations is that the controls are applied over only one face of the cube. In this paper, the method of moments is employed to establish spectral controllability for the above case (meaning that any finite combination of eigenfunctions is controllable). In the companion paper [S.S. Krigman, C.E. Wayne, Boundary controllability of Maxwell's equations with nonzero conductivity inside a cube, II: Lack of exact controllability and controllability for very smooth solutions, J. Math. Anal. Appl. (2006), doi:10.1016/j.jmaa2006.02.102] it will be established, by modifying the calculations in [H.O. Fattorini, Estimates for sequences biorthogonal to certain complex exponentials and boundary control of the wave equation, in: New Trends in Systems Analysis, Proceedings of the International Symposium, Versailles, 1976, in: Lecture Notes in Control and Inform. Sci., vol. 2, Springer, Berlin, 1977, pp. 111–124], that exact controllability fails for this geometry regardless of the size of the conductivity term. However, we will also establish in [S.S. Krigman, C.E. Wayne, Boundary controllability of Maxwell's equations with nonzero conductivity inside a cube, II: Lack of exact controllability and controllability for very smooth solutions, J. Math. Anal. Appl. (2006), doi:10.1016/j.jmaa2006.02.102] controllability of solutions that are smooth enough that the Fourier coefficients of their initial data decay at a suitable exponential rate.