AbstractWe introduce a numerical method for the solution of the time‐dependent Schrödinger equation with a smooth potential, based on its reformulation as a Volterra integral equation. We present versions of the method both for periodic boundary conditions, and for free space problems with compactly supported initial data and potential. A spatially uniform electric field may be included, making the solver applicable to simulations of light‐matter interaction.The primary computational challenge in using the Volterra formulation is the application of a spacetime history dependent integral operator. This may be accomplished by projecting the solution onto a set of Fourier modes, and updating their coefficients from one time step to the next by a simple recurrence. In the periodic case, the modes are those of the usual Fourier series, and the fast Fourier transform (FFT) is used to alternate between physical and frequency domain grids. In the free space case, the oscillatory behavior of the spectral Green's function leads us to use a set of complex‐frequency Fourier modes obtained by discretizing a contour deformation of the inverse Fourier transform, and we develop a corresponding fast transform based on the FFT.Our approach is related to pseudospectral methods, but applied to an integral rather than the usual differential formulation. This has several advantages: it avoids the need for artificial boundary conditions, admits simple, inexpensive, high‐order implicit time marching schemes, and naturally includes time‐dependent potentials. We present examples in one and two dimensions showing spectral accuracy in space and eighth‐order accuracy in time for both periodic and free space problems. © 2020 Wiley Periodicals LLC.