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Light induced degradation of polymers has drawn increasing interest due to the need for externally controllable modulation of materials properties. However, the portfolio of polymers, that undergo precisely controllable degradation, is limited and typically requires UV light. A novel class of backbone‐degradable polymers that undergo aerobic degradation in the presence of visible light, yet remain stable against broad‐spectrum light under anaerobic conditions is reported. In this design, the polymer backbone is comprised of 9,10‐dialkoxyanthracene units that are selectively cleaved by singlet oxygen in the presence of green light as confirmed by NMR and UV/vis spectroscopy. The resulting polymers have been processed by electrohydrodynamic (EHD) co‐jetting into bicompartmental microfibers, where one hemisphere is selectively degraded on demand.

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