Multi-shell diffusion MRI (dMRI) unlocks more expressive microstructural modeling than single-shell scans, yet its longer acquisition time hinders deployment in large-scale cohorts and time-constrained clinical settings. Synthesizing an unobserved shell from a single-shell input is fundamentally ill-posed and further complicated by protocol mismatch, where source and target gradient direction sets may not align. We propose DTI-SHNet, a single-to-multi-shell synthesis framework that operates in the real symmetric spherical harmonics (SH) coefficient domain and performs spatially aware volumetric regression. Given a source shell, we estimate diffusion tensor imaging (DTI) and use direction-agnostic parametric maps along with a brain mask as conditioning priors to guide a 3D U-Net regressor from source-shell to target-shell SH coefficients. To couple coefficient accuracy with signal fidelity, we introduce a signal consistency regularization that reconstructs signals on randomly sampled canonical directions from predicted coefficients and enforces agreement in the signal domain. Experiments on UK Biobank and Cam-CAN data for b=1000 to b=2000 dMRI synthesis show that DTI-SHNet achieves competitive visual quality compared to advanced methods, while better preserving downstream diffusion measures. Our code is available at https://github.com/xiaovhua/dti-shnet.

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