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3Enzymes are biological catalysts involved in crucial cellular processes such as signaling pathways, DNA replication, and protein expression. In biotechnology, enzymes are used for manufacturing biosensors, [1] medicines, [2] fuels [3] and foodstuffs. [4] A methodology for inactivating a target enzyme on demand could be useful for discerning the role of the biocatalyst in a particular cell function. [5] A light-triggered inactivation mechanism would be ideal for these applications since it would enable turning off the enzyme activity noninvasively and on demand. Current methods for controlling the activity of enzymes with light require the synthesis of photoresponsive enzyme substrates, i.e. a molecule that changes its conformation upon irradiation at a particular wavelength. [6] While this approach allows a fine control over the activity of a given enzyme, it can only be applied to those enzymes whose substrate can be synthesized in a laboratory. Furthermore, enzymes show exquisite specificity for the conversion of a particular substrate. This means that different lightresponsive molecules must be synthesized for each specific enzyme, which is very timeconsuming. Moreover, supplying synthetic substrates may be cumbersome in intracellular or in vivo studies, in which the photoresponsive molecules may need to permeate cell membranes and compete with naturally occurring substrates in order to inactivate the enzymes. In this context it would be highly desirable to find a generic methodology that allowed inactivating any target enzyme remotely regardless of its substrate specificity and in different biological scenarios, such as in the presence of other enzym...