Brutalist developments in London are weirdly polarised. Either they've been torn down because of chronic social problems like the Heygate estate, or they're Grade II listed and massively desirable like Trellick Tower, the Barbican or Rowley Way.
The Heygate estate is an interesting point. I used to live in the foursquares, a smaller equally deprived estate just to the east.
At the time of the "regeneration" (2000s) it was a toss up between a number of estates and the heygate. However because of its size and location the heygate was chosen
My estate was turned around, and I was lucky enough to live in the estate, not on it. I got to know some of the original residents(and still do).
There are two important things to note, Council housing is almost exclusively of a very high standard (bigger than new builds by ~10+ sqm) Compared to the slums described so vividly in the road to wigan pier, a paradise. (running toilets, windows, heating plaster, enough bedrooms for each kid)
Until a rule change in the late 70s, you had to have a job to be eligible for council housing. There were (and still are, more or less) residents associations that look after the running of the estate. Caretakers lived on site, towers had 24 hour concierges, and ne'dowells were evicted.
However, that was all taken away in favour of dumping problem families, outsourcing cleaning and upkeep (In some cases, one cleaner 2 hours a day costs something line £80k annually.)
In short, there is nothing wrong with the estate fabric (of the surviving estates) but how they are looked after, and who lives there. Grenfell is a shining example, a solid block that was subdivided and halfarsedly put in new gas mains.
By living _in_ the estate, I mean I turned up to the residents meetings, and participated in the governence of the estate. Council housing has been sold off, and represents a cheap, profitable rental income. Because of the high rate of change, they are socially and funtionally seperated from either leaseholders or council tenants.
When it came to regeneration/improvements, we were the one consulted, not the private renters.
If I missunderstood your question, here is some waffle:
An estate is a logical collection of dwellings, normally flats (but can be houses) that were commissioned and built by local governement for the express purpose of housing the employed working classes.
for example my estate was made up of four blocks of about 180 flats. Each block encloses a shared garden, with childrens play equipment.
It's important to know that the Barbican was built as luxury housing. Trellick or Alexandra Road were social housing and they still have a much broader social mix.
On one hand, I'm sure I would hate living in a city where everything looked like the Barbican. Yet, every time I'm there I'm awed by its strange beauty. It has such a strong identity.. it feels like walking inside a sculpture.
I found that one part of the feeling you describe comes from it being "organic" in an unusual way. It's easy to find any number of modern buildings that use "organic" shapes or materials (think curved or made from wood). However, they will still be boring and predictable inside and fit into a very boring street grid outside. Barbican is different: it's "brutalist" and as un-organic in its material as possible, but the structure itself is an unpredictable, multilevel maze where you don't know what awaits you around the corner. That provokes a very different feeling, more akin to a forest over the rolling hills than to a city. And it's built that way both inside and out, at least as far as public spaces are concerned.
I think that different kind of "organic" is why I love Barbican. There aren't many places that make me feel like a child exploring a new area, but Barbican is the best at that.