High aspect-ratio 2D materials are promising for solution-processed electronics, yet the factors controlling exfoliation remain unclear and relatively few solution-processed networks have been electrically characterized. Here we combine theory and experiment to show that electrochemical exfoliation of layered crystals with sufficient stiffness-anisotropy (in-plane/out-of-plane Young’s modulus ratio >1.7) yields high aspect-ratio nanosheets with intrinsic mobilities μ_NS = 20–75 cm²V⁻¹s⁻¹ across transition metal dichalcogenides and related alloys. Impedance spectroscopy indicates that solution-deposited networks can achieve junction-to-nanosheet resistance ratios (R_J/R_NS) as low as ~3, supporting theoretical predictions that μ_NS/μ_Net = R_J/R_NS + 1 and suggesting that further reductions in R_J will increase μ_Net toward the nanosheet limit (μ_NS). These networks display n-type, p-type, and ambipolar behaviour, with on/off ratios up to 10⁵ and mobilities μ_Net = 13 cm²V⁻¹s⁻¹. Here, we show that such high-performing 2D materials enable functional solution-processed circuits, including inverters, buffers, a 4-bit digital-to-analog converter, and a circuit capable of encoding and decoding 7-bit ASCII messages.

Networks of nanowires, nanotubes, and nanosheets are important for many applications in printed electronics. However, the network conductivity and mobility are usually limited by the resistance between the particles, often referred to as the junction resistance. Minimising the junction resistance has proven to be challenging, partly because it is difficult to measure. Here, we develop a simple model for electrical conduction in networks of 1D or 2D nanomaterials that allows us to extract junction and nanoparticle resistances from particle-size-dependent DC network resistivity data. We find junction resistances in porous networks to scale with nanoparticle resistivity and vary from 5 Ω for silver nanosheets to 24 GΩ for WS2 nanosheets. Moreover, our model allows junction and nanoparticle resistances to be obtained simultaneously from AC impedance spectra of semiconducting nanosheet networks. Through our model, we use the impedance data to directly link the high mobility of aligned networks of electrochemically exfoliated MoS2 nanosheets (≈ 7 cm2 V−1 s−1) to low junction resistances of ∼2.3 MΩ. Temperature-dependent impedance measurements also allow us to comprehensively investigate transport mechanisms within the network and quantitatively differentiate intra-nanosheet phonon-limited bandlike transport from inter-nanosheet hopping.