Bilingualism has been linked to structural adaptations of subcortical brain regions that are important nodes in controlling of multiple languages. However, research on the location and extent of these adaptations has yielded variable patterns. Existing literature on bilingualism-induced brain adaptations has so far largely overseen evidence from other domains that experience-based structural neuroplasticity often triggers non-linear adaptations which follow expansion-renormalisation trajectories. Here we use generalised additive mixed models (GAMMs) to investigate the non-linear effects of quantified bilingual experiences on the basal ganglia and thalamus in a sample of bilinguals with wide range of bilingual experiences. Our results revealed that volumes of bilateral caudate nuclei and accumbens were positively related to bilingual experiences in a non-linear pattern, with increases followed by decreases, in the most experienced bilinguals, suggesting a return to baseline volume at higher levels of bilingual experience. Moreover, volumes of putamen and thalamus were positively linearly predicted by bilingual experiences. The results offer the first direct evidence that bilingualism, similarly to other cognitively demanding skills, leads to dynamic subcortical structural adaptations which can be nonlinear, in line with expansion-renormalisation models of experience-dependent neuroplasticity.