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We demonstrate the features of the dipole and quadrupole resonant modes in extinction spectra of spherically anisotropic nanoparticles based on full-wave scattering theory. It is found that in a core–shell nanosphere, the introduction of spherical anisotropy in the core leads to a blue shift in resonant wavelengths for small nanoparticles, while, for large nanoparticles (core radius larger than 90 nm), the dipole resonant wavelength remains unchanged with the variation of spherical anisotropy. In addition, the peak strengths for the dipole and quadrupole modes are also studied. Numerical simulations show that the strong localization of electric fields can be further enhanced and tuned by adjusting the spherical anisotropy in the core. In contrast, the anisotropy introduced in the shell results in a blue shift for small nanoparticles but a red shift for nanoparticles with larger size. The tunability of plasmon resonant shifts in extinction spectra and tailored localization of enhanced fields are revealed.