Joshua Toole, 38, and a 24-year-old woman were arrested at Killarney Vale and Belmont shortly after 9am today during vehicle stops.
Officers had reportedly been investigating the supply of methylamphetamine through the NSW Central Coast and Hunter regions since April.
Police searched properties in Belmont North, Nords Wharf and Wadalba where they found more than two kilograms of methylamphetamine, $220,000 in cash, a gel-blaster, and electronic devices earlier today.
The methylamphetamine has a street value of $2 million.
A 43-year-old man was arrested during the search of the Belmont North home and a 42-year-old man was arrested at a workplace in Wyong.
All four people are expected to be charged, NSW Police said.
Investigations are continuing.