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A man in his 30s and a woman in her 20s were arrested at a property in Romford, Essex.
They were detained on suspicion of production of cannabis, holding a person in slavery of servitude, and possession of Class A and B drugs.
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Another man was arrested at the Romford address for immigration offences and remains in custody.
Two men, one in his twenties the other in his thirties, were arrested at a property in central Birmingham on suspicion of production of Class B drugs, possession of Class B drugs and immigration offences.
And as part of the investigation NCA officers also conducted searches at two properties in Burton on Trent.
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Four suspects were released under investigation and one remains in custody pending immigration enquiries.
NCA operations manager Neil Gardner said: “This is a complex investigation focused on a crime group believed to be using forced labour to produce cannabis.
“We know organised crime gangs often exploit the vulnerable to further their profits, both in the production of illegal drugs and in their distribution..
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“In some cases we have seen victims threatened and suffering extreme violence as the criminals exert control. This is why tackling modern slavery is a high priority for the NCA.”
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