A self-assembled 3D nanonetwork of Nickel and Nickel Oxide is synthesized by ultrashort pulsed laser through multiphoton ionization. The synthesized nanonetwork with tunable physiochemical property was investigated for cancer therapeutic and biomolecular sensing applications. In this thesis, the developed 3D nickel nanomatrix effectively regulated HeLa cancer cell adhesion and proliferation mimicking Extracellular Matrix (ECM). This behaviour explicitly demonstrated that the initial incubation period was devoted to baiting fibroblast and HeLa cells to proliferate upon the nanomatrix and subsequently the same nanomatrix exhibited cell trapping behaviour upon HeLa cells after an increased incubation period thereby controlling proliferation. The results brought new insight as to how HeLa cells behaved differently when compared to NIH3T3 fibroblast cells opening pioneering application in drug-free cancer therapy. To delve deeper into nickel nanonetwork for cancer therapy the laser ionization was manipulated to induce two distinct quantum theranosomes. Presently, quantum materials are limited due to 0D & 1D materials lacking biocompatibility resulting in coated materials with labelled tags for fluorescence excitation. The theranosomes mimicked tumor microenvironment by selectively accelerating the proliferation of mammalian fibroblasts cells while inducing cancer therapy. Furthermore, the theranosomes opened up label-free bioimaging probe for differentiating (HeLa & MDAMB-231) from mammalian fibroblast cells for cancer diagnostics. In-addition to label-free bioimaging, the development of an ultrasensitive biosensor for targeted biomolecule sensing was developed addressing the drawback faced with fluorescence imaging using Surface Enhanced Raman Scattering (SERS). We developed a SERS active nano-biosensor to detect chemical dye Crystal Violet (CV) and biomolecule glutathione(GSH). The Raman detection of crystal violet (CV) and glutathione (GSH) molecules was noted with 1 pM (1×10-12M) concentrations at (532 & 785nm) excitation wavelengths with an enhancement factor of 109, not been observed even in plasmonic materials. This extends the limit of detection (LOD), confirming suitability for chemical and biomolecular sensing. Additionally, the quantum confinement effect will result in an ultrasensitive sensor diagnosing and differentiating cancer cells from fibroblast cells. Based on the results in this thesis, the multifunctional feasibility of nano and quantum scale nickel structures arranged in 3D assembly for its direct application in cancer therapeutics, encompassing cancer bioimaging and diagnostics.