In this work, tung oil was utilised as a catalyst-free self-healing agent, and an in-situ polymerization process was applied to encapsulate the tung oil core with a poly(urea-formaldehyde) (PUF) shell. The conventional poly(ethylene-alt-maleic-anhydride) (PEMA) polymer was compared to a more naturally abundant gelatin (GEL) emulsifier to compare the microcapsules’ barrier, morphological, thermal, and chemical properties, and the crystalline nature of the shell material. GEL emulsifiers produced microcapsules with a higher payload (96.5%), yield (28.9%), and encapsulation efficiency (61.7%) compared to PEMA (90.8%, 28.6% and 52.6%, respectively). Optical and electron microscopy imaging indicated a more uniform morphology for the GEL samples. The thermal decomposition measurements indicated that GEL decomposed to a value 7% lower than that of PEMA, which was suggested to be attributed to the much thinner shell materials that the GEL samples produced. An innovative and novel focused ion beam (FIB) milling method was exerted on the GEL sample, confirming the storage and release of the active tung oil material upon rupturing. The samples with GEL conveyed a higher healing efficiency of 91%, compared to PEMA’s 63%, and the GEL samples also conveyed higher levels of corrosion resistance.

Tung oil (TO) microcapsules (MCs) with a poly(urea-formaldehyde) (PUF) shell were synthesized via one-step in situ polymerization, with the addition of graphene nanoplatelets (GNPs) (1–5 wt. %). The synergistic effects of emulsifiers between gelatin (gel) and Tween 80 were observed, with gel chosen to formulate the MCs due to its enhanced droplet stability. SEM images then displayed an increased shell roughness of the TO-GNP MCs in comparison to the pure TO MCs due to the GNP species on the shell. At the same time, high-resolution transmission electron microscopy (TEM) images also confirmed the presence of GNPs on the outer layer of the MCs, with the stacked graphene layers composed of 5–7 layers with an interlayer distance of ~0.37 nm. Cross-sectional TEM imaging of the MCs also confirmed the successful encapsulation of the GNPs in the core of the MCs. Micromanipulation measurements displayed that the 5% GNPs increased the toughness by 71% compared to the pure TO MCs, due to the reduction in the fractional free volume of the core material. When the MCs were dispersed in an epoxy coating and applied on a metallic substrate, excellent healing capacities of up to 93% were observed for the 5% GNP samples, and 87% for the pure TO MC coatings. The coatings also exhibited excellent corrosion resistance for all samples up to 7 days, with the GNP samples offering a more strenuous path for the corrosive agents.