The diversity of carbon materials makes it possible to prepare all-carbon electronic devices requiring components with different properties and functions. In this work, we fabricate an all-carbon solution-gated transistor (AC-SGT) based dopamine (DA) sensor with Nafion coated nitrogen and oxygen co-doped carbon yarn (Nafion/NOCY) as the gate electrode and graphene as the channel. The carbon materials in AC-SGT render the usage of a variety of strategies to improve its electrochemical sensing capability including the modification of the gate electrode and the modulation of the operating voltage. With a low gate-source voltage of 0.02 V as well as a low drain-source voltage of 0.05 V, AC-SGT manifests the outstanding DA sensing performances in terms of sensitivity, selectivity, limit of detection (3 nM, S/ N > 3), linear range (3 nM to 300 μM), long-term stability (over 30 days), and preconditioning time (60 s). Furthermore, a smartphone controlled portable sensing system integrated with AC-SGT is fabricated herein, which shows the excellent in vitro sensing capability of DA in urine, proving the potential of all-carbon transistors in smart wearable biosensors.