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In this monograph, we consider natural operations on directed graphs. And we find the connections between our operations on graphs and the groupoid-perations on "graph" groupoids. Remark that we cannot guarantee the (algebraic or categorial) groupoids generated by the grouopoid-operations; sum, product, quotient or complement; of graph groupoids are again graph groupoids. By defining suitable operations on graphs, we can conclude the groupoids generated by the groupoid-operations of graph groupoids are again graph groupoids; for example, the product groupoid of two graph groupoids...