They said they had found a significant clue, according to media reports.
Data from the plane’s voice recorder suggest Andreas Lubitz had deliberately started a descent while the pilot was locked out of the cockpit.
Germanwings flight 9525 from Barcelona to Duesseldorf crashed on March 24.
Several airlines have now pledged to change their rules to ensure at least two crew members are present in the cockpit at all times.
The revelations by the German police come after officers searched Andreas Lubitz’s flat in Duesseldorf and the house the 27-year-old shared with his parents in Montabaur, north of Frankfurt, late on Thursday.
A number of items were removed – including boxes and a computer – from the two properties.
“We have found something which will now be taken for tests. We cannot say what it is at the moment but it may be a very significant clue to what has happened,” the Daily Mail quoted police spokesman Markus Niesczery as saying.
However, police said the discovery was not a suicide note.
There were also unconfirmed reports in the German media that Andreas Lubitz had suffered from depression.
Meanwhile, German government officials said Andreas Lubitz was not known to the country’s security services.
Earlier, Carsten Spohr, the head of Lufthansa, the German carrier that owns Germanwings, said the co-pilot had undergone intensive training and “was 100% fit to fly without any caveats”.
Carsten Spohr said Andreas Lubitz’s training had been interrupted for several months six years ago, but did not say why.
The training was resumed after “the suitability of the candidate was re-established”, he said.
On March 26, Marseille prosecutor Brice Robin said the co-pilot appeared to want to “destroy the plane”.
Citing information from the recovered “black box” voice recorder, Brice Robin said Andreas Lubitz was alone in the cockpit just before the crash.
Brice Robin said there was “absolute silence in the cockpit” as the pilot fought to re-enter it.
Air traffic controllers made repeated attempts to contact the aircraft, the prosecutor added, but to no avail.
Passengers were not aware of the impending crash “until the very last moment” when screams could be heard, Brice Robin said, adding that they died instantly.
“We hear the pilot ask the co-pilot to take control of the plane and we hear at the same time the sound of a seat moving backwards and the sound of a door closing,” the prosecutor said.
Brice Robin said the pilot, named in the German media as Patrick Sonderheimer, had probably gone to the restroom.
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