Amanda Spielman says schools in London are not well enough supported when it comes to dealing with knife crime.
Ms Spielman says that schools do not have the ability to address the complex societal problems that lie behind the rise in knife violence.
She also says exclusions are not the root cause of the surge in knife crime.
"Children who carry knives almost invariably have complex problems that begin long before they are excluded," the watchdog says.
In a report, Safeguarding children and young people in education from knife crime - lessons from London, Ofsted looks at how more than 100 schools, colleges, and pupil referral units (Prus) in the capital are protecting children from knife violence in school, as well as how they teach pupils to stay safe outside of school.
The report, which follows a spate of fatal teenage stabbings, says knife crime needs to be tackled by various groups, including police, local authorities and policy makers.
It also says serious violence on school grounds is "extremely rare".
Ms Spielman says: "Schools simply do not have the ability to counter the deep-seated societal problems behind the rise in knife crime.
"Some schools are valiantly trying to fund school-based early help services or other services that were once provided for free.
"But we cannot allow responsibility for this to be landed on schools in the absence of properly funded local services."
The Ofsted report says the common denominator among young people involved in knife violence is their vulnerability.
"Almost invariably, these children have experienced poverty, abuse or neglect or are living within troubled families," it says.
"They may also experience social exclusion due to factors such as their race or socio-economic background.
"School leaders also told us that those involved were also more likely to be low attainers academically compared with their peers."
Ms Spielman also says schools are worried about damaging their reputation if they talk about the issue of knife crime openly.
"Many school and college leaders we spoke to were trying to educate children about the dangers of knife crime and the risks of grooming and exploitation by gangs.
"However, some are concerned that if they do this they will be seen as a 'problem school', and subsequently avoided by parents."
What does Ofsted recommend?
The report says:
- schools have very different ways of dealing with knives and teaching children about the risks and head teachers need more guidance about what works
- schools have inconsistent approaches to involving the police and there is an overall lack of clarity on when this is necessary, meaning children at some schools are more likely to be criminalised for their actions
- more clarity is needed on "managed moves", when a child is moved from one school or Pru to another, and the Department for Education should collect data on these, as it does on exclusions.