Multimodal neuroimaging allows for non-invasive examination of human brain structure and function across multiple scales. Precision neuroimaging builds upon this foundation, enabling the mapping of brain structure, function, and connectivity patterns with high fidelity in single individuals. Ultra-high field (UHF) neuroimaging, operating at magnetic field strengths of 7 Tesla or higher, increases signal-to-noise ratio and offers even higher spatial resolution. Here, we provide a multimodal Precision Neuroimaging and Connectomics (PNI) dataset, utilizing UHF 7T magnetic resonance imaging (MRI). Ten healthy individuals underwent a comprehensive MRI protocol, including T1 relaxometry, magnetization transfer imaging, T2*-weighted imaging, diffusion MRI, and multi-state functional MRI paradigms, aggregated across three imaging sessions. Alongside anonymized raw imaging data, we release cortex-wide connectomes from different modalities across multiple parcellation scales, and supply “gradients” that compactly characterize spatial patterning of cortical organization. Our precision imaging dataset will advance our understanding of structure-function relationships in the individual human brain and is publicly available via the Open Science Framework (https://osf.io/mhq3f/).