Abstract-Simultaneous recording of electroencephalographic (EEG) signals and functional magnetic resonance images (fMRI) has gained wide interest in brain research, thanks to the highly complementary spatiotemporal nature of both modalities. We propose a novel technique to extract sources of neural activity from the multimodal measurements, which relies on a structured form of coupled matrix-tensor factorization (CMTF). In a datasymmetric fashion, we characterize these underlying sources in the spatial, temporal and spectral domain, and estimate how the observations in EEG and fMRI are related through neurovascular coupling. That is, we explicitly account for the intrinsically variable nature of this coupling, allowing more accurate localization of the neural activity in time and space. We illustrate the effectiveness of this approach, which is shown to be robust to noise, by means of a simulation study. Hence, this provides a conceptually simple, yet effective alternative to other data-driven analysis methods in event-related or restingstate EEG-fMRI studies.