The quest for economically sustainable electrocatalysts to replace critical materials in anodes for the oxygen evolution reaction (OER) is a key goal in electrochemical conversion technologies, and, in this context, metal–organic frameworks (MOFs) offer great promise as alternative electroactive materials. In this study, a series of nanostructured electrocatalysts was successfully synthesized by growing tailored Ni-Fe-based MOFs on nitrogen-doped graphene, creating composite systems named MIL-NG-n. Their growth was tuned using a molecular modulator, revealing a non-trivial trend of the properties as a function of the modulator quantity. The most active material displayed an excellent OER performance characterized by a potential of 1.47 V (vs. RHE) to reach 10 mA cm⁻², a low Tafel slope (42 mV dec⁻¹), and a stability exceeding 18 h in 0.1 M KOH. This outstanding performance was attributed to the synergistic effect between the unique MOF architecture and N-doped graphene, enhancing the amount of active sites and the electron transfer. Compared to a simple mixture of MOFs and N-doped graphene or the deposition of Fe and Ni atoms on the N-doped graphene, these hybrid materials demonstrated a clearly superior OER performance.

Supercapacitors and transistors are two key devices for future electronics that must combine portability, high performance, easy scalability, etc. Graphene‐related materials (GRMs) are frequently chosen as active materials for these applications given their unique physical properties that are tunable via chemical functionalization. Up to date, among GRMs, only reduced graphene oxide (rGO) showed sufficient versatility and processability in mild media, rendering it suitable for integration in these two types of devices. Here, a sound alternative to rGO is provided, namely graphene acetic acid (GAA), whose physico‐chemical features offer specific advantages. In particular, the use of a GAA‐based cathode in a zinc hybrid supercapacitor (Zn‐HSC) delivers state‐of‐the‐art gravimetric capacitance of ≈400 F g⁻¹at a current density of 0.05 A g⁻¹. Conversely, GAA‐based LGT, supported onto Si/SiO₂, shows an ambipolar behavior in 0.1 mNaCl, featuring a clear p‐doping quantified by Dirac voltage higher than 100 mV. Such a device is successfully implemented in paper fluidics, thereby demonstrating the feasibility of real‐time monitoring.

Liquid‐gated transistors (LGTs) are versatile devices for low‐power electronics, in‐field sensors, and neuromorphic devices. Among functionalized graphene‐based materials, graphene acetic acid (GAA) has been successfully integrated into LGTs as a prototypical solution‐processable 2D material with controlled surface chemistry and a conductivity of 1.8 mS/m. Like other liquid‐phase exfoliated 2D materials, the printing of GAA networks into micropatterns on arbitrary surfaces represents a major challenge. To overcome this limitation, we leverage a dielectrophoretic‐based approach to fabricate GAA films with an average thickness of 470 nm. Our fabrication strategy offers several advantages: (i) high reliability (i.e. ≈ 100% success rate out of more than 25 fabricated devices); (ii) small amount of active material required (< 30 µL of a 0.2 mg/mL of GAA), (iii) high spatial‐resolution (i.e. the deposition efficiency scales inversely with electrodes distance), and (iv) no further post‐processing steps. Our GAA‐based LGTs exhibit lower channel resistance (10–30 kΩ) than drop‐cast counterparts, negligible gate leakage current (10–50 nA), and modest hysteresis. Moreover, hole/electron mobility of 10 ⁻¹ cm ² V ⁻¹ s ⁻¹ and a Dirac voltage close to −189 mV have been demonstrated. Furthermore, these devices exhibit a stable electrical response when exposed to air for 4 h and to continuous bias stress for 30 min.