relate neural activity with stimulus and action across multiple timescales-from millisecond-precise spiking patterns that represent sensory and motor information to longer-term neural plasticity that enables neural circuits to progressively adapt to changing environmental contingencies. [2,3] High-density silicon probes and microwire arrays [4][5][6][7] are valuable tools for large-scale recordings of neuronal activity at single-spike resolution and have been applied to show that perceptual learning involves distributed brain regions. [8,9] However, the mechanical mismatch between stiff probes and soft neural tissues can cause micromotion-related inflammatory responses and recording instabilities, [10][11][12] limiting their long-term use in basic and biomedical applications. Flexible probes, including injectable mesh electronics, [13] nano electronic thread, [14] and Neurotassel, [15] have been developed to reduce the mechanical mismatch between probes and tissues. These probes have shown greatly reduced micromotion and inflammatory responses in the brain, thus leading to improved long-term stability in neuronal recordings. However, the bending stiffness of micrometer-thick polymer substrates in these flexible probes is typically two orders of magnitude higher than that of nanofilm electrodes, making it a limiting factor in cellular-scale electrode-tissue interfacings. It is thus highly desirable to develop novel neural electrode technologies [13][14][15][16][17][18][19][20][21][22][23][24][25] that can enable intimate integration with neural tissues and stable tracking of neuronal activity over long terms.In this study, we develop free-standing nanofilm electrode arrays for intimate neural interfacings and stable neuronal activity tracking over long terms. To assist depth implantation into the brain, each NEA was encapsulated into a biodissolvable polymer carrier through elastocapillary selfassembly. After implantation into mouse brain, the high flexibility of free-standing gold nanofilms facilitated their intimate and innervated integration with neural tissues. As a result, chronically implanted NEAs could allow stable tracking of the same populations of neurons over months. This capability allowed us to study how the same neuronal populations in the dorsal striatum represent and update stimulus-outcome associations across multiple timescales during perceptual learning.Flexible neural electrodes integrated on micrometer-thick polymer substrates offer important opportunities for improving the stability of neuronal activity recordings during cognitive processes. However, the bending stiffness of micrometer-thick polymer substrates is typically two orders of magnitude higher than that of nanofilm electrodes, making it a limiting factor in electrode-tissue interfacings. Here, this limitation is overcome by developing self-assembled nanofilm electrode arrays (NEAs) that consist of high-density, free-standing gold nanofilm electrodes. Chronically implanted NEAs can form intimate and innervated interfaces with neural...