mainly due to the steep material development progress in the last 20 years and the resulting long cycle life (>1000 cycles), [3,4] which is especially crucial for devices charged at least one to two times a day. [5-7] However, despite its high theoretical capacity of 274 mAh g −1 , LCO only delivers a useable specific capacity of about 140 mAh g −1 at an upper cutoff voltage of 4.2 V (vs Li/Li +). [8-10] Hence, charging to higher cell cutoff potentials of 4.2-4.5 V has been a way to achieve higher specific energy. [11] However, at potentials above 4.5 V (x = 0.28), LCO shows a fast capacity fade, mainly due to instability of the layered structure and deleterious phase transition. [11,12] Cobalt dissolution, [9] oxygen loss, [13] and side reactions with the electrolyte [9] have also been shown to decrease lifetimes when cells are repeatedly charged to high potentials. Mitigating the issues with LCO at high potentials has attracted a lot of research interest and helped to improve the stability of LCO using surface modifications, including coatings, [14-18] and doping with a variety of elemental compositions. [18-20] Today, these efforts have led to LCO having the largest market share in terms of battery use for mobile consumer applications. [2,4] Besides offering high cycling stability for mobile consumer applications, another The ever expanding mobile consumer electronic market has accelerated the need for safe and efficient fast-charging approaches that improve the overall speed of battery charging without hastened deterioration of the battery performance. Herein, the impact of a resource inexpensive, physics-based, electrochemically optimized fast-charging algorithm (charging time < 2 h) for mobile devices is investigated. A critical difference in the amount and morphology of lithium deposits on the anode for cells fast-charged without an optimized algorithm is observed and found to be the main cause of capacity decay. An in-depth study of the LiCoO 2 cathode regions opposite to pronounced lithium deposits on the anode reveals a "mirroring" phenomenon, i.e., a frozen monoclinic phase, and inactivity to relithiation. In operando hard X-ray absorption spectroscopy reveals that degraded spots on harvested cathodes seem to be activated again and participate in the intercalation process when lithiated at low rates from lithium foil counter electrodes. On the other hand, tests at higher Crates , closer to the actual fast-charging rate, reveal only negligible oxidation state changes and therefore poor performance.