The bioorganometallic platinum(II) compounds PtU6 and PtU5 were designed by the conjugation of the corresponding uracil derivative and the organoplatinum(II) compound [4-octyloxy-(C^N^N)PtCl]. The single crystal X-ray structure determination of PtU6 revealed the formation of the dimeric structure through intermolecular hydrogen bonds between the uracil moieties of two independent molecules, wherein each hydrogen-bonded dimer was connected through Pt(II)–Pt(II) and π–π interactions. The tuning of the emission properties of the organoplatinum(II) compounds was achieved by changing the direction of hydrogen bonding sites and the molecular scaffold having two 2,6-dihexamidopyridine moieties as a complementary hydrogen bonding site for the uracil moiety, which depends on the regulation of the aggregated structures, to induce the Pt(II)–Pt(II) and π–π interactions.