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The realization of advanced optical fiber probes demands the integration of materials and structures on optical fibers with micro- and nanoscale definition. Although researchers often choose complex nanofabrication tools to implement their designs, the migration from proof-of-principle devices to mass production lab-on-fiber devices requires the development of sustainable and reliable technology for cost-effective production. To make it possible, continuous efforts are devoted to applying bottom-up nanofabrication based on self-assembly to decorate the optical fiber with highly ordered photonic structures. The main challenges still pertain to “order” attainment and the limited number of implementable geometries. In this review, we try to shed light on the importance of self-assembled ordered patterns for lab-on-fiber technology. After a brief presentation of the light manipulation possibilities concerned with ordered structures, and of the new prospects offered by aperiodically ordered structures, we briefly recall how the bottom-up approach can be applied to create ordered patterns on the optical fiber. Then, we present un-attempted methodologies, which can enlarge the set of achievable structures, and can potentially improve the yielding rate in finely ordered self-assembled optical fiber probes by eliminating undesired defects and increasing the order by post-processing treatments. Finally, we discuss the available tools to quantify the degree of order in the obtained photonic structures, by suggesting the use of key performance figures of merit in order to systematically evaluate to what extent the pattern is really “ordered”. We hope such a collection of articles and discussion herein could inspire new directions and hint at best practices to fully exploit the benefits inherent to self-organization phenomena leading to ordered systems.