Ismail Abdi, 24, was arrested on Wednesday after officers raided properties at South Melbourne, along with Tarneit, Truganina and Albion in Melbourne's west.
He has been charged with offences including intentionally causing serious injury and illegally possessing a firearm.
A 23-year-old man from Werribee in Melbourne's southwest was also arrested but released pending further inquiries.
Police arrested Abdi almost three weeks after a gunman wearing a white hazmat suit opened fire on a 76-year-old man who answered a knock at his front door on Canterbury Road in Middle Park on August 17.
He was shot in the leg and hospitalised but survived the attack, which was described as "brazen" by police.
Two women inside the home, aged 72 and 39, were uninjured.
In announcing the arrest, police said they seized a white Hyundai as part of their investigation.
Abdi, who is from Tarneit, faced Melbourne Magistrates Court on Wednesday evening via video link from police custody.
No application was made for bail and he was remanded in custody until November 29.
Abdi is also due to front court on an unrelated firearm charge earlier that month.
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