The functional organization of neural processes is constrained by the brain's intrinsic structural connectivity. Here, we explore the potential of exploiting this structure in order to improve the signal representation properties of brain activity and its dynamics. Using a multi-modal imaging dataset (electroencephalography, structural MRI and diffusion MRI), we represent electrical brain activity at the cortical surface as a time-varying composition of harmonic modes of structural connectivity. The harmonic modes are termed connectome harmonics, and their representation is known as the connectome spectrum of the signal. We found that: first, the brain activity signal is more compactly represented by the connectome spectrum than by the traditional area-based representation; second, the connectome spectrum characterizes fast brain dynamics in terms of signal broadcasting profile, revealing different temporal regimes of integration and segregation that are consistent across participants. And last, the connectome spectrum characterises fast brain dynamics with fewer degrees of freedom than area-based signal representations. Specifically, we show that with the connectome spectrum representation, fewer dimensions are needed to capture the differences between low-level and high-level visual processing, and the topological properties of the signal. In summary, this work provides statistical, functional and topological evidence supporting that by accounting for the brain's structural connectivity fosters a more comprehensive understanding of large-scale dynamic neural functioning.