In this paper, we study a class of partitions called unrestricted singular overpartitions with parameters \( k \) and \( i \) , which is an overpartition such that no part is divisible by k, and any single occurrence of a part congruent to \(\pm i \pmod {k}\) may be overlined. The number of all such overpartitions of \( n \) is denoted by \({\overline{Cu}_{k,i}}(n)\) . Previous studies have established several congruence properties for \({\overline{Cu}_{3,1}}(n)\) modulo 2 and 4, and \({\overline{Cu}_{4,1}}(n)\) modulo 2, 4, and 8. We extend these results by deriving new congruences for \({\overline{Cu}_{6,1}}(n)\) modulo 36, 48, and 64. In addition, we establish connections between unrestricted singular overpartitions and other partition families, including \((k,\ell )\) -regular bipartitions and overpartitions with \(\ell \) -regular nonoverlined parts.